Carl Court / Staff
In a letter to Corbyn, Tristram Hunt said he had found his time as an MP "intensely frustrating" following the party's defeat in the 2015 general election.
"The extraordinary privilege of serving in Parliament has proved both deeply rewarding and intensely frustrating," he wrote.
"The frustration came... with the inability to address [my policy priorities] and implement our policy programme following our defeat in 2015.
He goes on to cite Labour's struggle to respond to the "social, cultural and economic forces which have rocked mainstream social democratic and socialist parties."
Hunt will now resign his seat in Stoke-on-Trent Central, in order to become the new director of the Victoria and Albert Museum.
Hunt was a former leadership candidate and a leading member of the moderate wing of the Labour party. His resignation comes within days of Corbyn's relaunch of his leadership.
He was singled out last year by Corbyn's team as one of 14 Labour MPs who had undermined him. A list leaked to the Press Association quoted Hunt as describing Labour under Corbyn as being "in the s***." He reportedly faced deselection by left-leaning members of his local constituency.
Hunt's departure means that Labour faces another by-election test in an area that voted overwhelmingly to Leave the EU.
Labour currently holds a majority of 5,000 votes in Stoke on Trent Central. However, UKIP have a strong presence in the area, narrowly beating the Conservatives into second place in 2015.
Hunt's departure follows the resignation of fellow Corbyn-sceptic MP Jamie Reed. Reed's resignation means the party also faces a tough battle to hold onto his seat in Copeland, Cumbria.