Glass, who has represented North West Durham since 2010, was appointed shadow education secretary on Monday, in the wake of a string of resignations on the Labour front bench.
Yesterday she announced her intention to step down as an MP at the next general election. But today she announced on Twitter that she was quitting the role with immediate effect.
"It is with a heavy heart that I have today resigned as shadow secretary of state for education," she said.
"[It is] my dream job but the situation is untenable."
Her resignation followed a vote of no confidence by Labour MPs in party leader Jeremy Corbyn. The 172-40 vote followed a string of resignations from the shadow cabinet and calls for Corbyn to quit.
Yesterday Glass announced that she did not intend to stand again at the next election.
"Given that the election could come as soon as October 2016, I want to give the [constituency Labour Party] as much time as possible to get a new candidate in place to fight the election," a letter posted by Glass on Twitter stated.
"Whilst I had always intended to do no more than two terms in parliament, I have found the last six months very, very difficult," she added.
"The referendum has been incredibly divisive, it divided families and communities and I have found it bruising in many respects. It has had an impact on both me and my family as I am sure it has had on many others."
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