Force India announced that Sergio Perez will partner Nico Hulkenberg next season, leaving di Resta and team-mate Adrian Sutil without a seat.
Di Resta joined the team at the start of 2010 and spent he year as their reserve driver, alongside his duties in DTM.
He stepped up to a race seat in 2011, registering a best finish of fourth place in Singapore last year and in Bahrain in 2013.
'Just want to take this opportunity to thank @clubforce [Force India] for 4 great years,' he posted on his Twitter account.
'As a team we've come a long way in our time together.'
'But it's now time for a new challenge for me in the next phase of my career and I wish them all the best for the future.'
Di Resta remains an outside contender for one of the vacant seats at Sauber, although a return to DTM - where he won the title in 2010 - is the most likely option.