The Last Song actress was reported in September to be in final talks for a new version of the classic American crime story, to be produced by Smash's Craig Zadan and Neil Meron for A+E's History and Lifetime channels.
An insider disclosed to Gossip Cop this week that Cyrus recently chose to depart the project for unspecified reasons.
Producers have apparently already begun the search to recast the role of Bonnie Parker. It is also not known who will play Parker's lover Clyde Barrow.
Cyrus has not commented on this latest development.
Barrow and Parker were previously immortalised on-screen in the 1967 film Bonnie and Clyde, which starred Faye Dunaway and Warren Beatty as the duo.
Bonnie and Clyde earned a 'Best Supporting Actress' Oscar for Estelle Parsons and also won 'Best Cinematography'.
Watch a trailer for the 1967 Bonnie and Clyde below: