Wolff will take on the role of Private Adam Winfield, a US soldier who told his parents members of his platoon were murdering Afghan civilians, while Skarsgard will play Sergeant Deeks.
Dan Krauss' film is in pre-production, reported Contactmusic.
"When we first saw Dan Krauss' documentary, we were shocked by this story and blown away by his direction," a statement from producers Marty Bowen and Wyck Godfrey read.
"His film's scope and tension, combined with these morally ambivalent characters, made it irresistible to watch.