The 65-year-old actor will portray an FBI agent alongside Pfeiffer and De Niro, a mafia couple, who relocate to France under the witness protection programme, reported Contactmusic.
The Luc Besson directed film is based on Tonino Benacquista's book 'Badfellas'.
Besson has adapted the script and will also produce the film, which starts production in France in August.
Jones' has recently starred in blockbusters "Captain America" and "Men In Black 3". He will next appear opposite Meryl Streep in "Hope Springs", Steven Spielberg's "Lincoln" and Peter Webber's Japan-set drama "Emperor".
Meanwhile he is set to write, direct produce the indie film "The Homesman".