The Russian model will make her acting debut in the fifth instalment of the Bruce Willis action series, reports Variety.
It is currently unclear what role the star will take on in the project, which also stars Jai Courtney and will be set in her home country.
Vyalitsyna is perhaps best known for her work in the Sports Illustrated Swimsuit Issue series.
She also dated Maroon 5's Adam Levine after appearing in the videos for 'Misery' and 'Never Gonna Leave This Bed'.
The pair were together for two years before confirming their split in April.
Patrick Stewart has recently been rumoured for the role of a disgraced Russian general in Die Hard 5, while Sebastian Koch, Amaury Nolasco and Cole Hauser are also said to be among the supporting cast.
Max Payne's John Moore will direct with a script from Skip Woods.
A Good Day to Die Hard opens in cinemas on February 14, 2013.
In pictures: Bruce Willis starts filming A Good Day to Die Hard: