Over 80% have voted in favour of independence for Catalonia, after an informal, non-binding referendum according to officials.
Catalan leader Artur Mas hailed the poll "a great success" that should now allow a formal referendum.
"We have earned the right to a referendum. Once again Catalonia has shown that it wants to rule itself. I ask the people in the world, I ask the media and I also ask the democratic governments in the world to help the Catalan people decide its political future," Mas said.
Over 2 million people took part in the ballot, out of an estimated 5.4 million eligible voters.
The Spanish government had blocked an official referendum and dismissed the result of the vote.
"The government considers this to be a day of political propaganda organised by pro-independence forces and devoid of any kind of democratic validity," Spanish Justice Minister Rafael Catala said in a statement.