The latest instalment - titled Underbelly: Badness - will be set between 2001 and the present day and focuses on the story of crime boss Anthony Perish.
The Slap star Jonathan LaPaglia, who was nominated for an AACTA award earlier this year, will play Perish, with Matt Nable (East West 101) cast as Detective Inspector Gary Jubelin, head of the force who brought Perish to justice.
Aaron Jeffery and former Home and Away star Jodi Gordon will appear in supporting roles.
"Underbelly: Badness is a riveting and compelling story of a modern underworld figure that merged into the fabric of our community completely under the radar, and we are very proud to shine a light on this story and bring it to Australian audiences," Nine Network drama executives Jo Rooney and Andy Ryan said in a statement.
The previous series of Underbelly was set in the 1920s. Titled Underbelly: Razor, it starred Danielle Cormack and Chelsie Preston Crayford as rival vice queens Kate Leigh and Tilly Devine.
Preston Crayford was presented with the 'Graham Kennedy Award for Most Outstanding New Talent' at Sunday's TV Week Logie Awards.