Littrell, who has spent the past two seasons at Indiana, will replace Blake Anderson, who left North Carolina in December to become head coach at Arkansas State. UNC has yet to make an official announcement.
Littrell also coached tight ends and fullbacks at Indiana, two groups he's expected to oversee with the Tar Heels. He served as Arizona's offensive coordinator in 2011.
Indiana has promoted Kevin Johns to offensive coordinator. Johns has held a co-coordinator position with the Hoosiers and also coached wide receivers and quarterbacks.
Hoosiers coach Kevin Wilson, a former offensive coordinator at Oklahoma and Northwestern, said in a statement that he will maintain a major role in the team's offensive play calling and game plan.
James Patton will coach Indiana's tight ends and fullbacks after previously assisting with the defensive line and special teams.
The Hoosiers will hire a defensive assistant to replace Patton and maintain five assistants on defense for new coordinator Brian Knorr, Wilson said in a statement.
Indiana ranked ninth nationally in total offense (508.5 yards per game) and 16th in scoring (38.4 points per game) under Littrell in 2013.