Nick Clegg today ramped up the pressure on Bob Diamond by indicating he believed the Barclays chief executive should follow lead of the bank's chairman, Marcus Agius.
The Deputy Prime Minister said he had "no problem with more inquires" into what went wrong with the industry after Labour called for a Leveson-style investigation.
Mr Clegg sidestepped calls to directly demand Mr Diamond's resignation, insisting it was not for politicians to hire and fire bankers.
But, during a visit to a school in east London, he insisted the buck stopped at the top.
He said: "I'm like everybody else in this in that now that the chairman of Barclays has fallen on his sword and has taken responsibility for what has happened, everybody is asking when are the other senior people at the top of Barclays going to take responsibility for the things that happened on their watch.
"I don't think it is for politicians to individually hire and fire bankers, but I do think the buck stops at the top."
Mr Clegg accused Labour of "rank hypocrisy" for demanding a public inquiry into banking when it had launched a "prawn cocktail charm offensive" on the City during its time in power.
"I have no problem with the idea of more inquiries into what's gone wrong in our banking system," he said.
"We have had a whole lot in the past.
"We are now getting on with repairing the damage done to our banking system.
"I'm totally open to having more looks at what happened in the banking system.
"But I really do think it is rank hypocrisy of Ed Miliband and Ed Balls to trawl themselves round the television studios in this pious way, pretending that somehow they know what the answer is when it all happened on their watch.
"Ed Balls was on a prawn cocktail charm offensive in the City of London, sucking up to the banks, which is one of the reasons it's all gone wrong in the first place."
Mr Clegg later told CBBC Newsround British banks were now a "source of embarrassment and shame".
He said: "People at the top of these big banks who earnt lots of money, they had these big fat bonuses when things went well.
"They have also got to take the rough with the smooth, they have also got to be responsible when things go wrong on their watch."
He added: "The banks used to be the jewel in the crown of our country and now they are source of embarrassment and shame."