Cardoso was Brazil's president from 1995 to 2003 and is a leading figure in the PSDB, a centrist party opposed to Rousseff's left-wing Workers' Party.
He said anti-government protests last Sunday that drew three million people, according to police, showed Brazilians are demanding Rousseff's ouster.
"The streets cried out, 'Resign! Stop! Impeachment!'" he told newspaper O Estado de Sao Paulo.
Sixty-eight percent of Brazilians support impeaching Rousseff, up eight percentage points from February, according to a poll released Saturday.
The impeachment case, which is unrelated to the Petrobras scandal, is based on allegations she manipulated the government's accounts to boost public spending during her 2014 re-election campaign, and again in 2015 to mask the depth of the recession.
Cardoso, 84, had in the past voiced doubts on the wisdom of impeaching Rousseff, but said his opinion had changed "little by little."
"With the government's incapacity to function today... I think the path to follow now is impeachment," he said.
Rousseff's position is all the more precarious as the Petrobras scandal appears to close in on her.
She does not face charges, but chaired the company during much of the period in which investigators say executives colluded with contractors to overbill Petrobras by billions of dollars, bribing politicians and parties along the way.
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