Catalonia's regional leader has opened the door to a unilateral declaration of independence from Spain after police used batons and rubber bullets to disrupt a banned referendum in a show of force Catalan officials say injured more than 840 people.

Key points: Rubber bullets have been fired into crowds as ballot boxes were seized

Rubber bullets have been fired into crowds as ballot boxes were seized Madrid says it "did what it had to do" to shut down the illegal referendum

Madrid says it "did what it had to do" to shut down the illegal referendum A "yes" result is expected but the vote has already been blocked in Spain's courts

"On this day of hope and suffering, Catalonia's citizens have earned the right to have an independent state in the form of a republic," Carles Puigdemont said in a televised address.

"My government, in the next few days will send the results of today's vote to the Catalan Parliament, where the sovereignty of our people lies, so that it can act in accordance with the law of the referendum."

The Catalan Government said around 2.26 million people had cast a ballot in a referendum banned by Madrid to leave Spain on Sunday and 90 per cent of them had voted in favour of secession — this represents a turnout of around 42.3 per cent of Catalonia's 5.34 million voters.

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But Mr Puigdemont's comments followed a stern TV address by Spanish Prime Minister Mariano Rajoy, who maintained that the vote was illegal, and declared the region had failed to hold a referendum, while expressing hope "they give up on that path".

"We cannot allow that 40 years of harmony is thrown in the air through blackmail of the whole nation," he added.

"I hope that now they give up on the path that, as has been seen today, leads to nowhere."

Amid one of Spain's biggest political crises in decades, Mr Rajoy said that he would call all-party talks to "reflect on the future", but dialogue over Catalonia would be "within the law".

The comments from the Prime Minister came as Spanish riot police smashed their way into Catalonian polling stations to violently shut down the referendum, beating up voters and seizing ballot boxes.

Spanish police have been criticised for using batons and fired rubber bullets to crack down on protesters in Catalonia. ( AP: Manu Fernandez )

The law of the referendum, deemed unconstitutional by Madrid, foresees a unilateral declaration of independence by the regional parliament of Catalonia if the majority votes to leave Spain.

Nonetheless, the ballot in and of itself will have no legal status as it has been blocked by Spain's Constitutional Court, which ruled it at odds with the 1978 constitution that effectively restored democracy in Spain after the dictatorship of General Francisco Franco.

'We did what we had to do': PM Rajoy

Sorry, this video has expired Rubber bullets fired during police clashes with protesters in Catalonia

Police across the region hit people with batons, fired rubber bullets into crowds and forcibly removed would-be voters from polling stations in actions that were condemned internationally but described by the government as "proportionate".

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Catalan officials said overnight that over 840 people had been injured in the police crackdown, while Spain's Interior Ministry said 12 police officers had also been injured, and that they had been able to close 92 polling stations across the region.

In his speech, Mr Rajoy thanked security forces for upholding the law and doing their job, saying that "we did what we had to do", while also calling to meet with all Spanish political parties to discuss the country's future following the referendum.

Voting began at 9:00am local time, with the ballots closing 11 hours later at 8:00pm local time (5:00am AEDT) and the result of the referendum expected within 48 hours — but the disruption has plunged the vote's viability into chaos.

But despite the police action, some polling stations remained open, especially in areas under the supervision of the Catalan police force which adopted much milder tactics.

The Catalan Government said voters could print out ballot papers at home and lodge them at any polling station not closed down by police.

'Dreadful external image of Spain': Catalan leader

Sorry, this video has expired Catalonians vote in independence referendum despite police interference. (Image: AP)

Regional leader Carles Puigdemont accused Spanish authorities of using "unjustified, disproportionate and irresponsible" violence.

The batons, rubber bullets and violence used by Spanish police to prevent voting in what Spanish authorities have said was an illegal referendum had shown a "dreadful external image of Spain", Mr Puigdemont said.

"The unjustified, disproportionate and irresponsible violence of the Spanish state today has not only failed to stop Catalans' desire to vote … but has helped to clarify all the doubts we had to resolve today," he said.

The referendum has thrown the country into its worst constitutional crisis in decades and raised fears of prolonged street violence as a test of will between Madrid and Barcelona plays out.

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ABC/Reuters