Angelus (Buffy the Vampire Slayer)
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As Angelus, he was responsible for most of Angel's more reprehensible crimes including the killing of his family and of his village, the deaths of Holtz's family, and the turning of Holtz's daughter into a vampire who Holtz himself had to kill. Angelus himself was known for siring the vampires Penn, who indulged in his blood lust by being a serial killer, and Drusilla who Angelus drove insane before making her a vampire. He was also responsible for training William the Bloody who attributed Angelus as his "Yoda".
After Angelus tormented and killed a "beloved daughter" of a tribe of Gypsies, the Gypsies had their revenge by cursing him with a soul. Angelus became a prisoner in his own body and Angel re-emerged, wracked with guilt at the horrors he had committed. Angelus was forced to watch as Angel tried to achieve redemption, a unique form of torture for both Angelus and Angel.
Angelus's first appearance in the show's present-day was in Buffy's second season episode "Innocence". If Angel experiences one true moment of happiness, the Gypsy curse is lifted, he loses his soul, and Angelus re-emerges. After Angel and Buffy had sex, Angel's soul was taken from him.
After Angel became Angelus, he joined Spike and Drusilla. Angelus delighted in tormenting Buffy and her friends. His first main kill was Jenny Calendar, whose neck Angelus broke after she got too close to deciphering the Gypsy curse which would restore Angelus's soul. He then devoted his attention to destroying the world by attempting to awaken the demon Acathla.
Magic can be used to return Angelus's soul. In the second part of the Season Two finale "Becoming", Willow returned Angelus's soul with the use of an Orb of Thesulah, but Buffy was forced to send Angel to hell anyway, as it was the only way to prevent Acathla from sucking the world into a demon dimension. After a time in hell, Angel was eventually returned to the world by the Powers That Be.
Angel's soul was removed again, this time in Season Four of the spinoff series Angel. A shaman put Angel into a dream world which culminated in a moment of true happiness: This time, it was sex with Cordelia. Angel agreed to have his soul taken, because it was thought that only Angelus knew how to destroy The Beast, a fearsome demon who was terrorizing Los Angeles by blocking out the sun. Angelus ended up escaping, and his own ego drove him to kill The Beast. As Angelus, he fed off of, but did not kill, Lilah Morgan. He was captured with help from Faith, the "other" Slayer. His soul was again returned by Willow, whose crossover to Angel made one of the highlights of its fourth season. Angelus was not seen since then.
It has twice been assumed that Angel had reverted to Angelus, once in the Buffy season three episode "Enemies" and again in the Angel season five episode "Power Play". Both times, Angel had been merely duping his enemies into believing he had lost his soul, in order to gain their confidence and obtain vital information. Angelus appeared briefly on Angel, in the season one episode "Eternity", in which he was drugged with a substance which temporarily introduced happiness; however, after the drug wore off, Angelus was again imprisoned.