Carmen arrives in the year 2101 where she stops a heist of a powerful electro-magnet. Meanwhile, Zack and Ivy arrive at the future Acme Detective Agency where the wacky Future Chief doesn't recognize them. They try to prove who they are, but run into a few scrapes with the law. Eventually they meet up with Carmen in Africa. Although the detectives expose that she is a criminal, she escapes with the magnet and Zack and Ivy end up captured.

When Carmen attempts to steal several items having to do with military strategies, she is foiled several times by ""The Tigress,"" a thief with a lot of high-tech weaponery of her own. Meanwhile, Zack and Ivy rush into tell Chief something, but he doesn't listen until Carmen starts to listen in on their frequency, so now they can't tell Chief their secret. Every time from that point forward, when Carmen tries to steal something, the Tigress takes it first. The Tigress lures Carmen to Antarctica, where she reveals herself to be Ivy in disguise. Carmen was ambushed by Acme detectives and taken away, but escapes when she steals Ivy's CO2 boots Zack invented, and rockets away.

Zack and Ivy discover Carmen's underground training facility and go undercover as henchmen in training to try and nab Carmen. However, Carmen discovers them and leads them to a chamber that seems to have no way out. There is one way- an escape into time. Carmen created another time machine and uses it to escape. The detectives use a new Chronoskimmer that the Chief gives them and they trace where Carmen is heading- the future.

Zack and Ivy escape from the future and follow Carmen to Rome. There, the detectives are captured and are sentenced to fight each other in the Coliseum games. Luckily, they are spared from having to fight each other to the death. They escape, and discover Carmen's plan- she's going to steal the Coliseum! The detectives realize this is part of her plan to become ""the greatest thief of all time"" by stealing objects from the past, present, and future.

Somehow, the world's largest diamond, the Star of Africa, was stolen. The police are baffled and it's up to Zack and Ivy to figure this mystery out. They soon discover that one of Carmen's henchmen tried to double-cross her and keep the diamond for himself. With a little trickery of their own, the detectives recover the diamond.

It is reported that Carmen dies in a plane crash. The grief-stricken Chief is unable to help Zack and Ivy solve a series of clues that Carmen left behind to a final caper. The henchman who solves the most of them will be the new leader of V.I.L.E. Zack and Ivy manage to stop all of the thefts. They then travel to the site of Carmen's reported death to pay their last respects. Suddenly, a little bird delivers a message to ""look up."" When they do, they see Carmen was alive all that time. She had planned to fake her death to see who was worthy enough to take her place- and it turns out Zack and Ivy are the only ones who can!

Carmen's thefts all seem to follow a Wizard of Oz theme. While chasing after Carmen, Zack and Ivy discover that Carmen was an orphan. They trail her to the Golden Gate Girls' School which is about to be torn down. The detectives recover all the stolen objects except for the orphanage. Zack and Ivy see this theft as being almost justified though because it was about to be torn down and was the only home Carmen ever knew.

Zack and Ivy manage to capture Carmen in Hawaii. However, Zack loses his lucky rabbit's foot and begins to believe he's cursed with bad luck. Meanwhile, Carmen escapes and tries to teach her superstitious henchwoman, Hannah Lulu that there's no such thing as curses or ghosts. Hannah has a panic attack though when Zack and Ivy scare her at a supposedly haunted site. They manage to capture her but Carmen escapes. She leaves behind something Zack was glad to see again- his lucky rabbit's foot. He then gives it to Hannah and wonders if carrying around a special Hawaiian plant will give him better luck.

Carmen's reoccurring nightmare sends to her to seek the help of three Native American shamans to interpret it. Meanwhile, Zack, Ivy and a Native American detective named Billy ""Running Bird,"" track Carmen to Devil's Tower where the meaning of her dream is revealed. Though Carmen is captured, the shamans let her go. They do not want to go back on their promise- they would interpret her dream in exchange for the return of the items she stole from them and a promise to not detain her in any way.

Carmen gives herself a Christmas present by downloading The Chief. Only he's got a virus, and is losing his memory. He thinks that Carmen is still good, and that Zach and Ivy are thiefs.

Carmen steals parts of famous artwork to try to create her own personal masterpiece.

Zack and Ivy puruse Carmen to Ayer's Rock where she has brought items of mysterious origins together in an attempt to contact aliens.

Carmen's dream of landing on the moon inspires her to try and make it come true.

Carmen kidnapps two white lion cubs and sets up her own game preserve for them.

The Player challenges Carmen to a low-tech crime. Carmen accepts the Player's challenge and attempts to steal the Orient Express. Zack and Ivy need some help to solve Carmen's clues and are partnered with a gaucho detective named Armando.

Zack and Ivy are partnered with a Russian detective as they follow Carmen's game-like clues to Hawaii for a ""winner-take-all"" chess game.

Carmen figures out a way to steal musical talent and transfers it to her two talentless henchwomen. She decides to showcase her accomplishment in a concert inside the stolen Sydney Opera House

Carmen steals objects that have to do with literature such as Mark Twain's writing desk, Charles Dickens's inkwell, and a jungle ruin like the one that appears in the Jungle Book. They follow Carmen's clues to a remote hideaway in the Swiss Alps where they think Carmen was writing her memoirs. However, she was actually sending the detectives on a wild goose chase while Sara Bellum had tapped into Acme's files and stolen them all.

Carmen goes on a ""Wizard of Oz""-related heist.

Carmen goes back in time to steal obhgects that can change history. (i.e., the shoe on Paul Revere's horse, and the tea from the Boston Tea Party)

After recovering Ben's key, Zack and Ivy travel back to Boston and discover Carmen stole Paul Revere's horseshoe. They fail to recover it then and chase Carmen to England and prevent her from stealing the uncracked Liberty Bell. They manage to recover the horseshoe, but Carmen reminds them she can simply travel back through time and steal it again. Zack and Ivy follow her to Paul Revere's barn, but she gets away. Then the detectives return the horseshoe and history returns to normal. In the present day, Zack sets the Chronskimmer down for a moment and it disappears...

Zack creates a computer, the Zack Attack 20,000, which he believes will capture Carmen. However, when Carmen escapes with one of the treasures Zack had the computer protect, Ivy decides that she doesn't want to put her faith in it. The siblings go their own separate ways on this case, until Ivy is captured by Carmen.

Carmen and her band of pirates attempt to tske over a submarine.

When Carmen steals famous gifts from around the world, Zack and Ivy are puzzled- especially since her clues are in the form of a scavenger hunt. Suddenly, the detectives realize why Carmen is doing this. It's her birthday and she is stealing these famous gifts to give them to herself.

Carmen warns the Player that her next crime ""promises to be a real gem."" Soon he and the detectives discover what Carmen meant. She created a large diamond and uses it to cause an information traffic jam across Acme's frequencies.