A few weeks into her employment with the firm, Wesley Wyndam-Pryce picked her out of the secretarial pool to be Angel's new personal assistant, after Angel and his staff were given control of that branch of Wolfram & Hart.
Wesley apparently thought that a familiar face would be good for Angel.
Harmony was reunited with Spike when he returned, first as a ghost and then in corporeal form.
She tried to connect with him, and initially hoped to renew their relationship since he had a soul.
Cordelia insisted on giving Harmony a chance, despite the rest of the team growing increasingly frustrated with such habits as her popping gum or tearing pages out of books, and her references to her continued thirst for human blood did little to endear her to Angel either.
She accompanied the Angel Investigations team on a mission to investigate a new vampire cult — Wesley reasoning that she would be more likely to infiltrate the cult as some vampires could sense Angel's soul —, but soon betrayed them to their enemies.
The plan ended in an embarrassing defeat, especially when both Buffy and Xander considered the very thought of Harmony having minions to be amusing.
When Spike had both Buffy and Drusilla chained up, before making his declaration of love in front for the Slayer, Harmony intervened and tried to kill Spike with a crossbow as a form of liberation. Having departed Sunnydale, Harmony visited her old friend Cordelia in Los Angeles, without telling her that she had become a vampire.
Harmony tried to connect with Cordelia, but had difficulty controlling her demon side.
Ironically, she was also momentarily “in love” with Xander, like all other women of the city excepted Cordelia, because of a spell provoked by Amy Madison.
After Cordelia and Xander's breakup, Harmony tricked Cordelia into thinking that she has been re-admitted into the clique, only to humiliate and reject her.