Solo investigates a girl's school for the daughters of VIP's, including Miki Matsu, who has valuable secret information from her father, a Japanese diplomat. THRUSH agent Jason Sutro has gained the cooperation of the headmistress, Hester Partridge. The assistant dean, Verity Burgoyne, and all of the girl students have been brainwashed by Sutro to go into a trance upon hearing a recording of Brahm's Lullaby, and are ordered to kill Solo.

Solo is nearly killed by a superhuman, robotlike girl, Margo Hayward, one of an army of such devices invented by Dr. Pertwee for THRUSH. Illya joins up with Margo's ex-roommate, Andy Francis, and finds the laboratory, where a roomful of robots attack them.

In spoof of ""My Fair Lady,"" Solo is recuperating from a fall into a Venice canal, Illya teams with Mark Slate to uncover Baroness Bibi de Chasseur, a THRUSH money courier who has contact with the treasurer of THRUSH. They recruit a barroom entertainer, Rosy Shlagenheimer, an exact double, to impersonate her. The switch is made, but in the confusion the Baroness makes another switch and poses as Rosy, then finds herself falling in love with Slate.

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.

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 and Illya are assigned to protect Dr. Fazie Nahdi, a Gandhi like peace advocate, during a conference. Nellie Canford, a high school teacher, becomes linked to their efforts when her dental work begins receiving radio transmissions. Mahdi stays at the home of Brutus Thor, who is actually a THRUSH leader who is trying to kill him and Illya is trapped in a room full of toys that begin firing real bullets.

Solo and Illya protect Miranda Bryant, the wife of a presidential candidate, from a THRUSH plot to kidnap her, not realizing that she has already been kidnapped and replaced with a double Irina, an unwitting dupe of THRUSH. When they do catch on, the candidate, Senator Bryant and his aide Fairbanks, agree to play along but Fairbanks is the one behind the plot to put a THRUSH agent in the White House.

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.

An off-broadway actress is murdered during a phone call to U.N.C.L.E., and Solo and Illya investigate a connection between the show and a sudden malfunction in U.N.C.L.E.'s communications. The understudy, Janet Jarrod, takes over the lead role, and Illya joins the cast to find the jamming device.

While in Italy investigating a THRUSH plan to divert the Gulf Stream with heavy water, Solo finds himself eluding THRUSH guards, and ends up hiding under the bed of Pia Monteri. Solo escapes a shotgun wedding, the family feels Pia's honor has been compromised, and the girl's American uncles retired Prohibition-era gangsters ""Fingers"" Stilletto, Enzo ""Pretty"" Stilletto, and Federico ""Feet"" Stilletto are called. At the island headquarters of Louis Strago, Illya is tortured by Strago's sadistic female assistant, Miss Diketon. Solo joins forces with the Stilletto brothers to try and rescue him.

While in Italy investigating a THRUSH plan to divert the Gulf Stream with heavy water, Solo finds himself eluding THRUSH guards, and ends up hiding under the bed of Pia Monteri. Solo escapes a shotgun wedding, the family feels Pia's honor has been compromised, and the girl's American uncles retired Prohibition-era gangsters ""Fingers"" Stilletto, Enzo ""Pretty"" Stilletto, and Federico ""Feet"" Stilletto are called. At the island headquarters of Louis Strago, Illya is tortured by Strago's sadistic female assistant, Miss Diketon. Solo joins forces with the Stilletto brothers to try and rescue him.

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.

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.

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.

Scientist Adrian Cool spots a UFO approaching earth on his radar. His daughter, Coco is kidnapped, and Illya follows and he's captured also. Simon Sparrow, a power-mad millionaire, has faked the approaching UFO to secure power for himself as the representative on earth of the ""aliens"". Sparrow captures Solo and puts him in an experimental wind tunnel to kill him, but he is saved by Corinne. Coco develops a crush on Illya; while they are trying to stop Sparrow, they end up aboard his ""UFO"".

Dr. Rutter, after inventing antimatter, hides out in Suburbia under the name Willoughby because he fears his creation will be used destructively. Solo and Illya take a house there to find him. But THRUSH agent Miss Witherspoon also wants to find Rutter, and when Rutter sends his neighbor Betsy after some rare medicine from the pharmacist, Fletcher, the chase is literally on the find Rutter first.

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.

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.

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.

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.

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.

Jacqueline Midcult writes a best selling novel, The Pieces of Fate, which U.N.C.L.E. recognizes as being based on a series of missing THRUSH diaries. She loses her memory during a THRUSH attempt to kill her, and THRUSH agents Ellipsis Zark and Jody Moore, a book critic, plot to kidnap her and find out where she found the diaries. Solo and Illya take Jacqueline to a small town where her Uncle Charly and Aunt Jessie live, to try and revive her memory, but Zark and Moore follow and they all converge on the attic where the diaries are hidden at the same time.

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.

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.