Tens of thousands of people poured into the city waving the region's independence flag and brandishing the colours red and yellow.
This year's march aimed to be the biggest ever - and a protest against the Spanish government's tax laws.
Catalonia wants Madrid to review its tax agreement and provide a bailout.
Alfred Bosch, an MP from the Republican left of Catalonia, told the BBC: "All the flags I can see are the pro-independence flags of Catalonia with the lonely star right in the middle of the triangle.
"And everybody is wearing these flags. I have never seen so many pro-independence flags in my all life."
Protester Teresa Cabanes told Reuters: "This is a blow for the government. People like me came from everywhere. I don't think they were expecting something as big."
The huge volume of people overwhelmed the mobile phone network, which shut down for hours as a result, reports say.
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