The pair will play Harry and Zinnia Wormwood, who neglect and mistreat their gifted young daughter Matilda, portrayed in the new project by acting newcomer Alisha Weir.
Indian comedienne Sindhu Vee has also been added to the line-up of the Netflix film as librarian Mrs. Phelps.
The film is based on the classic Roald Dahl story of the same name, which inspired the 2010 stage show "Matilda the Musical".
Matthew Warchus, who directed the West End and Broadway versions of the production, will take charge of the new movie adaptation.
The beloved children's novel was previously made into a film in 1996, starring Mara Wilson as the titular character, alongside Danny DeVito, Rhea Perlman, Embeth Davidtz and Pam Ferris as the villainous Miss Trunchbull.
Graham is best known for playing Andrew "Combo" Gascoigne in the film "This Is England" (2006) and its television sequels "This Is England '86" (2010)," This Is England '88" (2011) as well as "This Is England '90" (2015). He also starred in the fifth season of the BBC One series "Line of Duty" (2019) as DS John Corbett and played Al Capone on the hit HBO series "Boardwalk Empire" (2010–2014). He will next be seen in the "Venom" sequel, "Venom: Let There Be Carnage", which is slated for a 2021 release.
Riseborough, meanwhile, received a BAFTA nomination for her portrayal of Margaret Thatcher in the television film "The Long Walk to Finchley" (2008), and won critical acclaim for her performances on the Channel 4 miniseries "The Devil's Whore" (2008) and "National Treasure" (2016). The English actress also landed a lead role on 2020's Italian series "ZeroZeroZero".