The Labour leader said voters could not trust what the Prime Minister says after he failed to tell the truth on taxes, small boats and NHS waiting lists.
In Tuesday's ITV debate, Mr Sunak said "independent Treasury officials" costed Labour's policies that "amount to a £2,000 tax rise for everyone".
But a top official at the department had warned ministers that the figure "should not be presented as having been produced by the civil service".
Labour last night said it showed Mr Sunak was "not just hopeless at his job, but a desperate liar" and claimed he had broken the ministerial code.
As he campaigned in Portsmouth, Hants, Mr Starmer said: "What you saw was a Prime Minister with his back against the wall, desperately trying to defend 14 years of failure, resorting -and it was an insight into his character - to lies. I don't say that lightly."
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