Similar to Doofenshmirtz, Charlene has the most personality differentiation from her original counterpart. As opposed to being good-natured and sarcastic, Charlene is very evil and intelligent, more so than her husband after he was defeated. At one time, she was able to formulate an attack at Danville Park as a successful diversion in order for Candace to bring Heinz to her penthouse in order to free him.
Just like her husband, Charlene is actually also willing to eliminate those that pose as some significant obstacle, such as blasting a grenade at the Firestorm Girls when they arrived at her lair, though this failed when the Firestorm Girls evaded the blast.
Charlene seems to care for her looks, evident when was battling Candace, she notices one of the freed agents cutting off her manicure, something which distracted Charlene long enough for Candace to defeat her in combat.
Despite her being a darker and more sinister version of the 1st Dimension Charlene, she does tends to have a certain flaw and lighter side: she reacted in shock when one of the freed agents messed up her manicure, something which distracted her long enough for Candace to defeat her in combat. In spite of her evil ways, she genuinely loves Heinz, since they had pretended to be divorced for financial advantages during Heinz's reign; she also truly cares for their daughter Vanessa, who was willing enough to help both her and Heinz escape from Resistance custody.
Charlene turns out to be an impressive shooter and a bo fighter, as she was able to briefly defeat Candace (who is also a bo fighter herself) in combat.
Just like her husband, Charlene is extremely intelligent, as she planted a fake divorce with him to ensure of their family's safety and finances just in case Doof would be overthrown and imprisoned. She was also able to initiate a series of attacks to trick the Resistance into freeing Doof.
It also seems that Charlene is able to understand and inherit some of Doof's skills in robotics, as she was the one who created the giant mechanical ants and turned several of O.W.C.A.'s animal agents into Animal Borgs with the same technology Doof used to create his Norm Bots and turn his nemesis Perry into Platyborg.
Charlene is only mentioned twice in the deleted scene "Vanessa Meets Doof" as part of the bonus feature of the DVD, supposedly being divorced with Heinz. When their daughter Vanessa berated her father for banishing her boyfriend Tony Marzulo, she decides to go back to her mother's place by taking her father's blimp keys to get there. As Vanessa leaves for Charlene's, Heinz tells her to tell Charlene that she had fun though.
In "Tales from the Resistance: Back to the 2nd Dimension", it is revealed that Charlene has her own penthouse during Heinz's reign, and had actually pretended to be divorced with Heinz for several financial advantages since she actually shares much of Heinz's evil. It is also revealed that she is responsible for the capture of many of O.W.C.A.'s agents (including Pinky the Chihuahua and Peter the Panda) and their transformations into cyborgs during Heinz's reign, similar to how Heinz defeated Perry the Platypus and transformed him into the cyborg he is now. Upon learning this, Resistance leader Candace Flynn decides to investigate the situation, and coerced Heinz into helping her. However, having expected this as part of her plan to free Heinz, Charlene has her cyborgs to trap Candace, Phineas, and Platyborg in her penthouse, planning to turn them into cyborgs. Charlene is also annoyed of Heinz focusing his attention on his childhood toy train Choo-Choo, so she just throws it away, resulting Heinz to go back to his evil ways. However, Ferb manages to free the three by pretending that he was turned into a cyborg by Charlene, allowing the Resistance to infiltrate Charlene's penthouse. As the Resistance manages to free all the agents of their evil programming with fedora hats equipped with magnetic deprogramming chips (except for Peter the Pandaborg), Candace engages into a bo staff fight with Charlene and defeats her. As Heinz and Charlene are about to be taken into custody, an arriving Vanessa tricks Candace into letting her have a moment with her parents, which allowed the Doofenshmirtz family and Pandaborg to escape in a hover car driven by Tony himself. As the notorious Doofenshmirtz family escape, Vanessa introduces Tony to Heinz and Charlene; the former recognizing him as the boy he banished earlier because of his interest towards Vanessa.