According to the Press Association, Crowe has signed on to play Javert, the police officer who is in pursuit of ex-convict Jean Valjean, played by Jackman.
"Even though I have dreamt about making the film of Les Misérables for over 25 years, I could never have imagined that we would end up with the dream director Tom Hooper, and the dream cast of Hugh Jackman and Russell Crowe as the two great protagonists Jean Valjean and Javert," producer Cameron Mackintosh told PA.
"Not only were they born to play these roles vocally, but they thrillingly inhabit this great score," he added.
The film's screenplay has been adapted from Victor's Hugo's original 1862 novel by Gladiator screenwriter William Nicholson.
Anne Hathaway, Amy Adams, and Rebecca Hall are currently competing for the female lead role of Fantine.
Les Misérables is being targeted for release in cinemas on December 7, 2012.