The 62 year-old succeeded Andre Villas-Boas at the helm of the Ligue 1 outfit last March, and guided it to a second-place finish behind champion Paris Saint-Germain in his only full season in charge.
Yet just weeks after earning Champions League qualification, the former Albiceleste boss is on his way after reportedly growing frustrated with a lack of transfer activity and ambition from the club.
"[We] would like to sincerely and warmly thank the work of Jorge Sampaoli," read an official club statement. "We are satisfied with the progress made and the emotions experienced together, but following a long reflection, the two parties [...] have agreed to put an end to this stage [of their careers].
Club president Pablo Longoria will now begin a search for a successor to Sampaoli, who leaves with 36 wins from 67 games in charge, and with a season still to run on his contract.