In Africa, Professor Kenton has developed a superman formula which he has been using on the natives, hoping to build an army with which to conquer all of Africa. Premier Khufu resists the use of the drug on his people. Illya meets up with Harry Blackburn, a shady safari guide, and Marsha Woodhugh, who is searching for her lost sister, a Tarzan like woman named ""Girl"" who has captured Solo.

A dying man carrying a partial film with the secret of Project Quasimodo, a miniature atomic bomb, gives only one clue to finding the rest of the film: the name of Marvin Klump, inept car salesman. THRUSH agents Rodney Backstreet and Beirut capture Klump. Solo and Illya, with the aid of Klump's sister Heather, follow them first to the Alps, them back to the U.S.,where the answer to the puzzle lies in a cemetery.

Illya goes to the Himalayan country of Chupat to protect the high lama, but is shot by ""Calamity"" Rogers, an American rodeo star. Solo is sent to find Illya, and learns that the prime minister has kidnapped the real successor to the throne and intends to install his own son instead. An entranced girl, Amra Palli tries to kill Solo after being brainwashed by the prime minister.

Solo and Illya must protect Premier Georgi Koz, a Khrushchev like European leader, on a visit to New York, Priscilla Worth is befriended by Loz and she takes him to a school for Santa Clauses run by Francis X. O'Reilly where just one of a series of assassination attempts against him must be thwarted by the two U.N.C.L.E. agents.

In Greece, Illya tries to recover stolen U.N.C.L.E. documents, but they fall into the hands of Stavros, a Greek bandit, who has ambushed Illya, thinking he is his daughter Kira's convict husband, Manolakas returning from prison. Kita is in love with Nico instead, and Solo and Illya must resolve the love triangle in order to retrieve the documents.

THRUSH agent L.C. Carson uses an Indian reservation as a front for his plan to assemble a hydrogen bomb, and kidnaps the tribe's chief, High Cloud, to ensure cooperation. Solo arranges for the Chief's daughter Charisma to return, but she ends up being kidnapped along with Solo and Illya, who is disguised as an Indian. Solo and Illya, along with a band of young Indian warriors on Motorcycles, encircle Carson and his men and try to stop them before its too late.

President Nasasos Tunik visits Paris. His assistant, Malanez, is determined to persuade the president that the French are his enemy, and arranges for various embarrassing and insulting incidents to occur. Solo and Illya are assigned to see that the visit goes smoothly, but Tunik falls in love with Candyce, and Malanez plans to disgrace Tunik by framing him in a plot to steal the body of Napoleon from his tomb.

Solo and Illya find that THRUSH agent Colonel Picks has developed exploding apples, which will be used to trigger a nuclear stockpile. Nina Lillette, a pretty hillbilly girl, latches onto them for excitement. Illya joins a picking crew at the farm, but he is buried alive in a tunnel with the volatile apples.

Solo and Illya visit the laboratory of Dr. True, who has discovered how to extract gold from seawater. But Dr. True dies from a poison given him by THRUSH agent Randolph, and Randolph also kills his wife Amanda. The gold extraction formula was distributed in portions by True to his daughters, in inscriptions on a photo of himself. Solo and Illya meet Sandy True, who accompanies them to Rome, to find her half sister Margo, now unhappily married to the destitute Baron de Fanzini to London, to find the next sister Imogen, who has been arrested by a Constablefor indecent exposure and finally the Alps, to find Yvonne, who is breaking off an unhappy relationship with Karl Von Kesser. But after decoding the message in Japan, Solo, Illya and Sandy are captured by Randolph and taken to THRUSH central for execution.

A THRUSH code is hidden in a dress pattern, and Solo and Illya go to the garment district and encounter the design shop of two down on their luck designers and their model Ramona and the cutter who has a crush on her, Jerry. THRUSH also tries to retrieve the garment, but Ramona keeps forgetting where she left it.

Solo and Illya are responsible for the security during Waverly's upcoming address to his alma mater, but the campus is seething with protest. Illya joins the demonstrators, and meets Minerva Swight, the daughter of the dean. The head of the board of regents, Jonathan Trumble, is a THRUSH agent, and he hires campus agitator Gregory Haymish to try and kill Solo and Illya, while Trumbull's THRUSH superior, Number 24, undergoes plastic surgery so he can impersonate the dean during the ceremony and kill Waverly himself.

Frank Cariago, the U.S. head of a crime syndicate, is under pressure from Uncle Giuliano. Cariago decides to buy a movie production directed by Sheldon Veblan so his girlfriend, Ginger Laveer can have the starring role. But the picture is a disguised plan to drop a bomb on the family's biggest rival-Las Vegas.

Solo and Illya go to Algiers to obtain a rare old book containing a THRUSH code from Pierrot La Mouche who has stolen it from his boss, Colonel Hamid. But La Mouche has a high price he wants U.N.C.L.E. to help him obtain Janine whom he is in love with.

Investigating the shipment of a tidal-wave machine by THRUSH, Illya ends up aboard a merchant vessel run by Captain Morton. Morton is obsessed with his past disgrace in a court martial, and the crew is on the verge of a mutiny, which Illya leads just as THRUSH arrives to take possession of the device.

Solo and Illya visit the laboratory of Dr. True, who has discovered how to extract gold from seawater. But Dr. True dies from a poison given him by THRUSH agent Randolph, and Randolph also kills his wife Amanda. The gold extraction formula was distributed in portions by True to his daughters, in inscriptions on a photo of himself. Solo and Illya meet Sandy True, who accompanies them to Rome, to find her half sister Margo, now unhappily married to the destitute Baron de Fanzini to London, to find the next sister Imogen, who has been arrested by a Constablefor indecent exposure and finally the Alps, to find Yvonne, who is breaking off an unhappy relationship with Karl Von Kesser. But after decoding the message in Japan, Solo, Illya and Sandy are captured by Randolph and taken to THRUSH central for execution.

In Rome, American tourist Darlene Sims becomes the unwitting carrier of a perfume atomizer with a secret formula. THRUSH uses a suave ladies man Cesare Guardia to charm Darlene, but he falls in love with her in the process.

Solo and agent Andreas Petros (Robert Wolders) are sent to the island of Ibos, where the Technological Hierarchy for the Removal of Undesirables and the Subjugation of Humanity has been spending huge amounts of money on some unknown project. Solo, posing as a visiting THRUSH official, meets Dr. Killman (John Larch), the head of the project, and Marnya (Barbara Luna), who reveals that Killman is working on an earthquake device, as the real THRUSH emissary arrives.

Solo and Illya travel to the Caribbean to help Dr. Delgado, who is under a voodoo curse and in a zombielike trance thanks to the local dictator, El Supremo, and his chief of police, Captain Ramirez. The U.N.C.L.E. agents are assisted by Suzy, an American hairdresser whom El Supremo will not let leave the island. They eventually turn to voodoo queen Mama Lou to turn the tables on him.

Lucho Nostra and a group of criminals take over a tiny European country, Ingolstein, because it has no extradition treaty. Prince Frederick is afraid to kick them out, so Solo convinces princess Vicky to return and do so, only to find that she cannot because the treasury has been replaced with IOU's to Nostra for the prince's gambling debts. Nostra arranges for permanent protection by forcing a marriage between Vicky and one of his henchmen, Artie King, but the two actually do fall in love. King duels Nostra, with the fate of the country riding on the outcome.

THRUSH agent Abbot Simon takes over the monastery at St. Thomas to use the mountain location to aim a new laser gun at a long distance target the Louvre in Paris. Solo visits the area and meets Andrea Fouchet, and together they try to stop Simon before he destroys the world's greatest art treasures.

A dissatisfied THRUSH collaborator tips U.N.C.L.E. off to a new deadly hiccup gas. A pendant he wears leads Illya to Greenwich Village and an art gallery run by Mark Ole, a THRUSH agent. Starving artist Sylvia Harrison joins Illya, who is nearly suffocated at the hands of a foam producing machine.

Solo goes to Sweden to obtain a new suspended animation device from Dr. A.C. Nilson, but the device and its inventor are taken by THRUSH. The doctor's daughter Neila helps Solo find him, and the doctor's assistant, Inga Anderson also feigns cooperation but is actually working for THRUSH agent Heinrich Beckmann. Beckmann uses the device to invade U.N.C.L.E.'s Scandinavian headquarters, and only Solo has a chance to stop him.

Brothers Simon and Peter Sweet both rival THRUSH leaders vying for promotion, do not realize that the toy hula doll they possess has an extremely powerful new U.N.C.L.E. explosive inside that is activated by heat. As the outside temperature rises, Illya and Solo try to recover it with the help of Wendy Thyme. Solo poses as a representative of THRUSH Central, but Mama Sweet a real member of THRUSH Central appears on the scene.

Solo and Illya go to India to help Suzanne de Serre, a French botanist trying to find out why the jungle is dying and local natives are disappearing. Prince Panat and Drusilla Davina, along with Colonel Quillon, are systematically using a chemical to destroy the jungle and kidnapping natives to work in the jewel mines for the prince.

Illya parachutes out of a plane carrying THRUSH code documents, but lands in the desert at an abandoned Foreign Legion post run by Captain Basil Calhoun (Howard Da Silva). Illya is accompanied by a stewardess, Barbara (Danielle DeMetz) while Solo races to find them before THRUSH does.