Gerald branched out into his acting career as Charles Young, his first appearance on The Jamie Foxx Show for 2 episodes with "Just Don't Do It" where Jamie and his mother (Jo Marie Payton) decided to marry him. In January 2001, Gerald appears again in the series finale "Always and Forever" where Jamie (Jamie Foxx) and Fancy (Garcelle Beauvais) got married and sang the opening ceremony at the wedding and joined by fellow singers Gladys Knight and Marilyn McCoo.
Gerald also sung lead vocals in two songs on the 2002 film documentary "Standing in the Shadows of Motown" - the story of The Funk Brothers. Levert performed "Shotgun" and "Reach Out I'll Be There".
Levert wrote and produced songs for other artists such as, Barry White, Stephanie Mills, Teddy Pendergrass, James Ingram, The Winans and The O'Jays.
Gerald Levert lend his vocals on Jim Brickman on the song "My Angel", for Brickman's 2006 album entitled “Escape.” Levert was posthumously featured on former group mates Keith Sweat's "Knew It All Along" and Johnny Gill from the singer's “Til the Morning album”.
On November 10, 2006, Gerald Levert was found dead in his bed at his Newbury home when a cousin tried to wake him. Initial reports stated that Levert had died of an apparent heart attack. Shortly before his death, Levert completed work on what would be his final studio album, “In My Songs”
On December 7, 2006, it was announced that Levert, along with soul legend Chaka Khan, gospel singer Yolanda Adams, and R&B crooner Carl Thomas were nominated for a Grammy in the category of Best R&B Performance by a Duo Or Group With Vocals for their collaboration on "Everyday (Family Reunion)", a song from the soundtrack of Tyler Perry's Madea's Family Reunion.
In February 2007, an autopsy report conducted by the Cuyahoga County coroner's office concluded that Levert's death was caused by a fatal combination of prescription narcotics and over-the-counter drugs. The drugs in his bloodstream included the narcotic pain relievers Vicodin, Percocet, and Darvocet, along with anxiety medication Xanax and two over-the-counter antihistamines. The autopsy also revealed that Levert had pneumonia. The official cause of death was acute intoxication, and the death was ruled accidental. Gerald Levert was only 40 years old.
Following the disclosure of Gerald Levert's cause of death, a family spokesman stated that all the drugs found in Gerald's bloodstream were prescribed to the singer. Gerald was taking the pain medication because of chronic pain from a lingering shoulder problem and surgery in 2005 to repair a severed Achilles tendon.