In 2002, Church released Prelude, a compilation drawn from her first four albums. The British release of Tissues and Issues in 2005 signalled a major shift in her career from classical crossover to pop, with Church performing much of her own original material. Church and Sony ended their contract in 2006, and she turned her attention to raising children. Between 2006 and 2008, Church hosted her own television program on Channel 4, The Charlotte Church Show, which offered sketch comedy, interviews, and music. She won several comedy awards for her work in this venue. Other television appearances included guest roles on Touched by an Angel and Heartbeat, and several specials. Church has also appeared in film, with a performance in Craig Ferguson's I'll Be There.
Church's second pop album, Back to Scratch, was released in 2010, and an EP, entitled One, appeared in 2012, promoted on a U.K. tour.
She has published two memoirs, Voice of an Angel (My Life So Far) and Keep Smiling.