The Justified star will appear alongside Kurt Russell, Peter Sarsgaard, Richard Jenkins and Jennifer Carpenter in the S Craig Zahler-helmed project.
Bone Tomahawk tells the story of four men who set out on a mission to rescue a group of captives from a band of savages that live beyond the border of civilisation.
Olyphant will play a clean-cut gunslinger who moves to the frontier to satisfy the dark urges that lie beneath his exterior, Deadline reports.
The actor will also reprise his role as US Marshal Raylan Givens in the fourth season of FX's Justified, which debuts in January.
Bone Tomahawk begins shooting in New Mexico in the spring.
Watch a teaser for season four of Justified below: