Ms Rayner's comments follow the success of the Prime Minister in yesterday evening's confidence vote.
Speaking outside Parliament, she said: “When you lie to the public and when you break your own laws, then the minimum standard you should expect is the Prime Minister to resign."
Ms Rayner has been a vocal critic of the Prime Minister after revelations of lockdown rule-breaking surfaced in the Sue Gray report.
She added: “I’ve heard ministers out today saying: ‘Oh we’ve got to move on, this draws a line under it.’
"It really doesn’t. Number 10 was the most heavily-fined property in the whole of the United Kingdom.
“That is a damning indictment and Boris Johnson should be ashamed of himself to think he can continue when other people lost loved ones and were not able to say goodbye to them.
“It was a damning indictment of his own peers and many MPs within the Conservative Party were pretty clear that they think he’s done a disgraceful thing.
“I think, you know, he’s mortally wounded.”
Labour MP Angela Rayner said Boris Johnson was "mortally wounded" Dominic Lipinski
Prime Minister Boris Johnson survived a no confidence vote yesterday Leon Neal
Sir Keir Starmer and Angela Rayner received questionnaires from Durham Constabulary, Labour confirmed, as the force investigates a gathering in party offices in April last year.
Both the Labour leader and his deputy have said they will stand down if fined by police.
Ms Rayner continued her statement, voicing her opinion on the Prime Minister's stint in office, reflecting on the cost of living crisis, NHS waiting lists and travel chaos.
She said: “I think it’s been clear over the last couple of months he’s not dealing with the cost of living crisis, the NHS waiting lists, he’s not delivered on the hospitals that he promised that they were going to get, the travel chaos people have seen, passport chaos, the whole of the Home Office, all the departments have not been able to deal with issues that real people are facing at the moment because they’ve been too fixated on trying to save Boris Johnson. He cares about one thing and that’s himself.”
When probed as to whether Labour would stop calling for Mr Johnson’s resignation now the confidence vote had been held, Ms Rayner said: “We’ve got the answers to the problems that the country faces at the moment, but the country will not move on while Boris Johnson the liar, the cheat and the law-breaker is continuing as Prime Minister, because it sets the standard for the future of our democracy.
“If we allow a prime minister to continue in office when he smirks and laughs and has taken the public for fools and lied and broken his own laws, well there has to be a line that is drawn, and I think the public won’t move on until Boris Johnson is gone.”
The vote of no confidence yielded 359 votes, with 211 Conservative MPs marking they had confidence in Boris Johnson.
Ms Rayner replied to questioning on the MPs that voted in support of the Prime Minister, saying: “At the end of the day the British public can see that some of those Conservative MPs voted against not lying to the British public, they voted against their interests and to save the skin of Boris Johnson, to save their own skin because they know that they’re tanking in the polls at the moment.
“The public have the power to remove Boris Johnson. He may think that he’s bought himself a bit of time, but people never forget that they didn’t get to say goodbye to their loved ones. The British public do not like liars, cheats and people that break the law.
Boris Johnson leading Cabinet today Leon Neal
“And I think that he is going to get absolutely hammered if he tries to have another general election on that basis.”
Labour leader Sir Keir Starmer made a statement following the announcements of the success of the Prime Minister.
He said: “The choice is clearer than ever before: Divided Tories propping up Boris Johnson with no plan to tackle the issues you are facing.
“Or a united Labour Party with a plan to fix the cost-of-living crisis and restore trust in politics.
"Labour will get Britain back on track.”
Sir Keir added how the PM was “utterly unfit for the great office he holds” and accused Tory MPs of ignoring the British public.
He stated: “The Conservative Government now believes that breaking the law is no impediment to making the law.”