- Video report by ITV News Correspondent Emma Murphy
Some 844 people were injured in clashes with the police as Catalans attempted to cast ballots in a disputed independence referendum.
Police fired rubber bullets at protesters and forcefully removed voters from polling stations as they attempted to stop Sunday's referendum.
The Spanish Interior Ministry said 92 polling stations were closed by illegal referendum and three people, including a minor, have been arrested for crimes of disobedience and attacking police.
Sunday's vote follows days of rallies and protests as separatists insisted they would go ahead with the controversial referendum on the region's independence from Spain, despite the authorities' declaring the "illegal" vote would not be allowed.
Some 33 police officers were also injured in the clashes.
The mayor of Barcelona Ada Colau has called for Spanish Prime Minister Mariano Rajoy to step down following the violent police response.
The deputy prime minister of Spain said the government had intervened with "firmness and proportionality", adding the Catalan government has behaved with "absolute irresponsibility" in holding a referendum.
Footage emerged on Twitter of police officers attacked firefighters who had been protecting people trying to vote.
FC Barcelona's Spanish league game against Las Palmas was played without fans at the Camp Nou Stadium, after the club unsuccessfully tried to get the game postponed.
Barcelona made the closed-doors announcement with less than a half hour to kickoff, with thousands of football fans already waiting outside the stadium.
Despite police being ordered to stop ballots being cast, queues had began forming outside polling stations in the early hours of Sunday morning.
Preliminary results showed 2.26 million people - of a registered Catalonian electorate of 5.3 million - had voted in the referendum, with 90% backing independence.
Supporters of independence - including parents and children - occupied schools which were among the 2,315 buildings designated to be used as polling stations, camping in them overnight to ensure they remained open.
Catalan officials had said voters would be allowed to cast ballots at any polling station, rather than a designated one as previously announced, as many locations have been sealed off by police.
Police broke glass and used bolt cutters to force their way into one building being used as a polling station near the city of Girona, after voters attempted to barricade themselves inside.
Polling station workers inside the building reacted peacefully and broke out into songs and chants as the police closed down the vote.
Huge rallies and protests have taken place in the days prior to the vote.
Spain's Constitutional Court suspended the independence vote more than three weeks ago, but Catalonia's regional government is pressing ahead with it and urging registered voters to take part.
Spain's foreign minister said that the Catalan government's plan is anti-democratic and runs "counter to the goals and ideals the European Union" is trying to advance.