As the United Kingdom election campaign resumed on Monday, Corbyn told a crowd in Carlisle, northern England, that Theresa May had cut police numbers during her time as Home Secretary, and repeated his pledge to recruit 10,000 new police officers, including armed officers.
Asked a second time if he wanted the PM to quit, Mr Corbyn said: 'We've got an election on Thursday and that's perhaps the best opportunity to deal with it'.
However, Mrs May also served as Home Secretary for the duration of the Coalition government from 2010-2015, during which time cuts to police numbers and funding formed part of Chancellor George Osborne's austerity.
With the general election only three days away, Mr. Corbyn said he would like to see Mrs.
At an election campaign event in London, Mrs May refused to say whether cuts to police numbers under her watch should be reversed after the head of the Metropolitan Police called for more resources in the wake of the London Bridge attack.
May called the snap election on June 8 in a bid to strengthen her hand in negotiations on Britain's exit from the European Union, but has come under criticism for her election campaign, both over its style and substance.
He tweeted this morning: "Theresa May responsible for security failures of London Bridge, Manchester, Westminster Bridge".
The Labour leader's comments came as Mrs May's record as home secretary, when police numbers fell by nearly 20,000, was under the spotlight following the second terror attack during the election period.
"That's not leadership", May said.
Mrs May said: "The Commissioner of the Metropolitan Police has said that the Met is well resourced, and they are, and that they have very powerful counter-terrorism capabilities and they do".
Liberal Democrat leader Tim Farron also criticised Mrs May for her record on policing.
The Conservative premier, speaking in central London on Monday, accused Corbyn of "boasting" about opposing every single counter-terror law.
"That's not leadership - that's an abdication of leadership".
Mr Corbyn was also asked by ITV News if he held Ms May "in any way" responsible and if cuts to the police contributed to the London Bridge atrocity.
"One leader who has opposed the use of shoot to kill, and given cover to the IRA when they bombed and shot our citizens - and who now, in the midst of an election campaign, wants to do all he can to hide or deny those views".