More than 500 people have been injured as riot police shut down polling stations on the day of the controversial independence referendum in Catalonia.
Officers were seen stamping and kicking protesters as they stormed buildings and seized ballot boxes.
Footage captured in the village of Sarria de Ter in the province of Girona showed authorities using an axe to smash down the doors of a polling station where Catalan president Carles Puigdemont was due to cast his vote.
And in Barcelona, the region's capital, officers fired rubber bullets at thousands of protesters demonstrating against their votes being denied.
At least 460 people have been hurt in the clashes across Catalonia, the city's mayor said, while Spain's interior ministry said at least 11 police officers had been injured.
And tens of thousands of fans have been banned from attending FC Barcelona's football match with Las Palmas as part of a protest against the violence.
Spain's Constitutional Court has suspended the referendum and the central government says it is illegal.
But regional separatist leaders pledged to hold it anyway and called on the area's 5.3million eligible voters to show up to cast their ballots. oday Mr Puidgemont condemned the Spanish government's crackdown. He said: 'Police brutality will shame forever the Spanish state.'
But the Spanish deputy prime minister Soraya Sáenz de SantamarÃa said officers in Catalonia are acting 'in a proportionate manner'.
She added that the Catalan government 'has behaved with absolute irresponsibility' by going ahead with the referendum. Police have been cracking down for days, confiscating millions of ballots and posters.
Tensions have been rising across the country over the planned vote, with thousands marching in Madrid to protest against the separatists' attempt to break up their nation, demanding that Catalan leaders be sent to jail.
In Barcelona, the capital of Catalonia, thousands more took to the streets to urge their prosperous region to stay inside Spain.
Spain's foreign minister said on Saturday that the Catalan government's plan is anti-democratic and runs 'counter to the goals and ideals' of the European Union.
'What they are pushing is not democracy. It is a mockery of democracy, a travesty of democracy,' Alfonso Dastis said.
He said some pro-independence groups are 'adopting Nazi-like attitudes by pointing at people that are against that referendum and encouraging others to harass them'.
Shock
FC Barcelona condemened the violence on the streets as it announced that its game today would be 'played behind closed doors'.The club has long supported Catalonia's right for a vote on independence, without throwing its weight behind the yes or no camp.
It said in a statement: 'FC Barcelona condemns the events which have taken part in many parts of Catalonia today in order to prevent its citizens exercising their democratic right to free expression.
'Given the exceptional nature of events the Board of Directors have decided that the FC Barcelona first team game against Las Palmas will be played behind closed doors following the Professional Football League's refusal to postpone the game.'
The club's president Josep Maria Bartomeu said: 'It wasn't done for security, the security was guaranteed.
'We have done it behind closed doors so that everyone can see our opposition at what is happening.'
It comes after it emerged that Las Palmas players would be wearing Spanish flags on their shirts to show the club's support for a united Spain.
This morning in Barcelona, police forcefully removed a few hundred would-be voters from a polling station at a school.
Daniel Riano was inside when the police busted in the building's front door.The 54-year-old said: 'We were waiting inside to vote when the National Police used force to enter, they used a mace to break in the glass door and they took everything.
'One policeman put me in a headlock to drag me out, while I was holding my wife's hand. It was incredible. They didn't give any warning.'
Ferran Miralles said a crowd scuffled with police outside as they formed a tight perimeter around the door. Miralles said: 'They were very aggressive. They pushed me out of the way.'
Elsewhere in the city, police have arrested several people outside the Treball voting centre amid scuffles on the street. Officers dragged some of the protesters away and detained them.
Why do some in Catalonia want independence?
Catalonia is one of Spain's wealthiest and most industrialised regions. The region has its own language and a distinct culture which leads many Catalans to consider themselves as being from a separate nation to Spain.
Independence movements have existed in Catalonia for centuries but Spain's financial woes in recent years following the 2008 financial crisis have exacerbated support for sovereignty.
Many Catalans believe they are paying more to the central government than they are getting back.
Why does the Spanish government want to stop a referendum?
The central government is vehemently opposed to the independence group with officials describing it as an 'evil' threat to Spanish democracy.
Catalonia represents 16 per cent of the country's population and accounts for 19 per cent of its GDP and 25 per cent of its exports. If the region was to vote for independence it would cause difficulties for the economies of both areas.
New borders would also immediately impact jobs and business on both sides. An independent Catalonia would not be a member of the European Union which would affect its current trade routes with member states..
The interior ministry said this afternoon that police have closed 79 of about 2,300 polling stations that the Catalan government has authorised to stage the referendum. It added that three people had been arrested, , including a young girl, for disobedience and assault.
Earlier today, Catalan government spokesman Jordi Turull said that voting was underway in 96 per cent of the voting centres.
People began arriving before dawn to join parents, children and activists who have been occuping polling stations across the region with the aim of preventing police from shutting them down.
'I have got up early because my country needs me,' said Eulalia Espinal, a 65-year-old pensioner who started queuing with around 100 others outside one polling station, a Barcelona school, in rain at about 5am. 'We don't know what's going to happen but we have to be here.' 'This is a great opportunity. I've waited 80 years for this,' said 92-year-old Ramon Jordana, a former taxi driver waiting to vote in Sant Pere de Torello, a town in the foothills of the Pyrenees and a pro-independence bastion.
He had wrapped his wrists in Catalan flags, among 100-150 people who gathered at a local school that had been listed as a polling station, ready to block any police from entering. A tractor also stood guard, though no police had yet arrived.
Meanwhile, in Madrid, several hundred people have staged demonnstrations in favor of Spanish unity and against the referendum.
Some 300 people gathered Sunday in the city's Plaza Mayor square, waving Spanish red and yellow flags and chanting slogans.
Half the crowd then moved to the city's emblematic Sol square and staged a second rally in front of the regional government's headquarters.
The protesters applauded police standing guard outside the building in a show of support for Spain's security forces. Separatist groups told people to hold activities in schools over the weekend to dodge the orders to vacate.
Some of the Catalans who are defying the court orders say they want to send a strong message of displeasure with central authorities.
Activist Augsti Gil said there were no ballots or ballot boxes in Barcelona's Joan Fuster high school, where more than a hundred people have joined another hundred who spent the night occupying the designated polling station.
Joaquim Bosch, a 73-year-old retiree, was at Barcelona's Princep de Viana high school, where a crowd of 20 people was growing.
He said: 'I have come to vote to defend the rights of my country, which is Catalonia.'