On Sunday, at a speech in Carlisle, Mr Corbyn had highlighted that 20,000 people officers had been cut while Ms May was Home Secretary between 2010 and 2016.
It follows the third terror attack to hit Britain in just over three months. On Saturday seven people were killed and 49 injured at London Bridge when attackers rammed a van into pedestrians before stabbing revellers in bars in the nearby Borough market.
While Mr Corbyn said the election on Thursday was “perhaps the best opportunity” to remove the PM from her post, he also backed calls for her to resign, telling ITV: "Indeed I would, because there's been calls made by a lot of very responsible people on this who are very worried that she was at the Home Office for all this time, presided over these cuts in police numbers and is now saying that we have a problem - yes, we do have a problem, we should never have cut the police numbers."
Mr Corbyn was pressed on the Prime Minister’s position after David Cameron’s former policy guru demanded she resigned for “security failures” that led to the terror attacks in Westminster, Manchester and London Bridge.
Steve Hilton, who left Downing Street in 2012, posted reports relating to an alleged suspect of Saturday’s attack, before adding: “Theresa May responsible for security failures of London Bridge, Manchester, Westminster Bridge.
“Should be resigning not seeking re-election.”
Commenting on newspaper reports that appeared to attribute some responsibility to the security services, he went on: “Theresa May blame shifting again. Her spin doctors attack MI5, but she was in charge of them for years.”
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.
He replied: "The primary responsibility for this lies with those who did it, they killed people in cold blood in a disgusting and appalling way and there's no words other than total condemnation.
"On the issues of policing - the Government has been warned repeatedly about police cuts, and the Police Federation and many others [have said] how 20,000 have gone down over the past seven years.
"We've said we'd put 10,000 back immediately and also increase the number of security officers that are available, because clearly intelligence is a very important part of this.
"It's also very important to have a message of bringing communities together and that is something I always give very strongly at all of my events."
At an election campaign event in London, Ms May, however, defended her record, adding: "Cressida Dick has said that the Metropolitan Police are well resourced - and they are, she has said they have very powerful counter-terrorism capabilities - and they do.
"We have protected counter-terrorism policing budgets, we have funded an uplift in the number of armed police officers."
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