The first Latin American Pope toured Rio de Janeiro in an open car and then met President Dilma Rousseff at the state governor's palace.
After he left, police fired tear gas to disperse anti-government protesters, reports the BBC.
The Argentina-born pontiff is in Brazil to attend the Roman Catholic World Youth Day festival.
In a speech soon after his arrival, he urged young Catholics to "make disciples of all nations".
"I came to meet young people coming from all over the world, drawn to the open arms of Christ the Redeemer," he said at the governor's palace, referring to Rio's famous vast statue of Jesus.
"They want to find a refuge in his embrace, right near his heart to hear his call clearly and powerfully."
About an hour after the welcoming ceremony, police fired stun grenades and tear gas against the demonstrators outside the palace.
It was the latest rally against what the protesters described as endemic government corruption across the country.
But some were also unhappy about $53m (£34m) in public fund being spent for the pontiff's visit.
In a separate development, the military said a homemade explosive device had been discovered at a shrine between Rio and Sao Paulo that the Pope is due to visit on Wednesday.
The device at the Shrine of Our Lady of the Conception of Aparecida was described as being "of low power" and was destroyed.
As Pope Francis disembarked from the Alitalia plane in Rio's airport earlier on Monday, he was welcomed by President Rousseff to cheers and applause from the waiting crowd. A choir sang an anthem linked to Youth Day and he was presented with a bouquet of flowers.
The Pope waved before being taken by motorcade to the centre of Rio, where thousands of pilgrims have gathered.
Source: BBC
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