Barclays should double the sum it pays to sponsor cycling projects in London to give more back to the community, Mayor Boris Johnson has said.
It was "good that Barclays coughed up £25m, quite frankly", said Mr Johnson, before adding: "I think they could cough up another £25m."
The bank would neither confirm nor deny if it had been asked for more money.
In an interview with BBC One's The Politics Show London, Mr Johnson was asked if he had already demanded the cash.
"I won't conceal it from you that I have," he said.
He "sincerely" hoped the bank would pay it, he added.
"And they should - let me tell you why. Because these people have received substantial sums of money from the taxpayer to keep the whole banking industry afloat."
Mr Johnson said banks were important to London and he would be "the last politician in Britain who's willing to say a word in favour of financial services".
The companies generated hundreds of thousands of jobs and "£31bn worth of tax" each year, he said.
"Like them or loathe them, we need them."
But it was important for a greater share of banks' earnings going to "the community that surrounds them", he said.
The full interview with Boris Johnson can be seen on The Politics Show on BBC One in London on Sunday 27 February at 1200 GMT.
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