Carl returns to his former allies in the Grove Street Families gang, working with his brother Sweet (Faizon Love), and fellow gangsters Ryder (MC Eiht) and Big Smoke (Clifton Powell) to reestablish Grove Street as the predominant gang in Los Santos. Carl is also forced to assist Tenpenny and Pulaski with several jobs, as well as helping his neighbor OG Loc, a wanna-be gangster rapper with no talent, get started with his music career by ruining the career of prominent rapper Madd Dogg (Ice T).
Shortly before a gang battle, Carl receives a call from his sister Kendl’s boyfriend Cesar Vialpando (Clifton Collins, Jr.), who shows Carl the vehicle involved in his mother’s shooting being escorted by Big Smoke, Ryder, a group of Ballas, and Tenpenny. Carl is too late to save his brother from being ambushed and is arrested and dumped in the San Andreas contryside to assassinate a witness threatening Tenpenny and Pulaski. Meanwhile, Ryder and Big Smoke, now openly in league with the Ballas, take over Los Santos, flooding it with crack cocaine.
Tenpenny has Carl work with the aged marijuana farmer hippie "The Truth" (Peter Fonda) in preparation to discredit a DA. In the meantime, the similarly exiled Cesar sets Carl up to assist in a robbery spree with his cousin Catalina and joining in underground street races. Through these races, Carl meets the blind Triad leader Wu Zi “Woozie” Mu and wins the deed to a garage in San Fierro from Catalina. With help from The Truth, Carl works to convert the garage to a chop shop.
Besides performing jobs for Tenpenny, Carl insinuates himself into the Loco Syndicate, Smoke and Ryder's supplier. Carl eventually assassinating the Syndicate leaders, killing Ryder, and blowing up their crack factory. He also helps Woozie fend off a rival San Fierro Vietnamese gang, the Da Nang Boys.
Carl is contacted by the presumed-dead Loco Syndicate leader Mike Toreno (James Woods), who reveals he's a secret government agent and agrees to secure Sweet's release from jail in return for Carl's help.
Later, Carl is invited by Woozie to become a partner in the Four Dragons Casino in Las Venturas, where they are facing harassment from the Mafia-run Caligula's Palace casino. To displace the Mafia, they begin planning to rob Caligula's. Through The Truth, Carl meets music producer Kent Paul (Danny Dyer) and through him Caligula's manager Ken Rosenburg (Bill Fichtner), under pressure for support from the three Liberty City families. When Salvatore Leone (Frank Vincent) comes to Las Venturas to take over all of Caligula's for himself he takes Rosenburg, Kent Paul, and Maccer hostage, but Carl helps them escape under the guise of helping Salvatore. Whilst working for Salvatore Carl is sent back to Liberty City in order to take out a mafia family operating at Saint Mark's Bistro. Only the front of the bistro and the background viewable from the front were made from GTA III. The interior of the bistro was made from scratch. After final planning Carl and Woozie carry out their heist, taking millions of dollars from Salvatore's Casino. After the heist Carl receives a phone call from an enraged Salvatore who repeatedly tells Carl he's, "Dead!" along with threats of murdering his friends and family. Carl mocks Salvatore and hangs up. Salvatore isn't heard from again for the rest of the game.
Meanwhile Tenpenny and Pulaski, now under indictment, try to kill Carl, but Carl manages to kill Pulaski. Carl also saves the fallen Madd Dogg from killing himself, becoming his manager, and reestablishing him in Los Santos. Shortly afterwards, Sweet is finally released and has Carl once again help him restore Grove Street.
Tenpenny goes to trial for several felonies, but the charges are dropped for lack of evidence, as – thanks to Carl – all the prosecution's witnesses are either disgraced, missing, or dead. Tenpenny's release sends anger and shock throughout Los Santos, triggering the in-game rendition of the 1992 Los Angeles Riots.
During the riots Sweet manages to track down Big Smoke who is living in a fortified crack fortress. Carl breaks through all of the defenses and kills Big Smoke in a shootout only to be confronted by Tenpenny who steals all of Big Smoke's drug money and escapes in a fire truck. Carl and Sweet pursue Tenpenny through the streets of Los Santos until Tenpenny loses control and crashes off a bridge, landing at the entrance of the Grove Street cul-de-sac. Tenpenny manages to crawl free of the wreckage before collapsing. As Tenpenny is dying Carl considers shooting him, but Sweet stops him, saying that they shouldn't leave evidence that Tenpenny was killed instead of it just being an accident.
In the aftermath Carl's family and friends arrive at the Johnson house for a meeting. Madd Dogg announces that he's received a gold record for his new album. Cesar also proposes to Kendl. As his friends and allies celebrate their success, Carl turns to leave. When asked where he's going, he replies, "Fittin' to hit the block, see what's happening."
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