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More than 2.2 million ballot papers were counted, out of 5.3 million eligible voters, the regional government later said, suggesting a turnout of less than 50 per cent.
About 90 per cent were in favour of independence, with about 8 per cent for the "no" camp and blank and void papers accounting for the rest.
Results will be forwarded "in the coming days" to the Catalan parliament "so that it may implement" a referendum law that obliges it to declare independence within 48 hours of a "yes" victory, Puigdemont said.
He also accused Spain of writing "a shameful page in its relations with Catalonia" and urged the European Union to hear out Catalan concerns.
"The European Union can no longer continue looking the other way," he said.
Some 844 people were hurt in clashes with police, according to Catalan health authorities, as officers in riot gear raided dozens of public buildings to prevent them from being used as polling stations.
Catalans had occupied the buildings before the weekend in a bid to keep them open.
"We had to do what we had to do," Spanish Prime Minister Mariano Rajoy said from Madrid. "Today there was no self-determination referendum in Catalonia," he said, and "democracy prevailed because the constitution was upheld."
Calling the referendum a "mockery of the very essence of democracy," Rajoy thanked judges, prosecutors and police, and claimed to have the full support of the EU and the international community, despite criticism from some politicians and high-profile figures.
Earlier, Puigdemont accused Spanish police of responding to "ballot boxes, ballot papers and schools" with "batons and rubber bullets." Such "police brutality will forever shame the Spanish state," he said.
Social media was filled with images of officers in tense stand-offs with crowds. Some people could be seen being dragged away by officers wearing helmets and carrying batons; others were injured and carried away in stretchers.
Spanish opposition leader Pedro Sanchez, of the socialist PSOE, said his country's territorial integrity "is at risk," while the radical left Podemos party and Barcelona Mayor Ada Colau called for Rajoy's resignation.
Rajoy said he would address parliament on Monday and summoned crisis talks between all parties represented in Madrid, including Catalan separatists. He said he would "never close any door" to dialogue, "but always within the bounds of the law and of democracy."
"Crowd control instruments" were used in only one of 70 raids, Interior Minister Juan Ignazio Zoido told broadcaster La Sexta. His ministry said on Twitter that 33 Spanish police officers were injured.
Zoido confirmed that the Catalan police, or Mossos d'Esquadra, asked "in writing" for Spanish counterparts to intervene in certain situations. The Mossos' willingness to carry out Madrid's anti-referendum orders had been in doubt.
Voting started at 9 am and ended on time at 8 pm (0700-1800 GMT). In one Barcelona school that served as a polling station, large crowds defended the building from the threat of police incursions, and as its gates were shut, people broke into the Catalan national anthem.
In the central Placa de Catalunya, where secessionists usually hold their rallies, the Yes camp set up a stage with four banners flagging up Catalonia's ambitions. They said: "Hello Republic, Hello World, Hello Europe, Hello New Country."
Catalan authorities prepared more than 2,300 polling stations. By 6 pm, Spanish police had managed to close only 319 of them, or less than 14 per cent of the total, Catalan government spokesman Jordi Turull said.
Voter registration was at times conducted manually as the Catalans' use of an online census was repeatedly sabotaged by Madrid. Long queues formed outside referendum sites, and some voters were moved to tears as they cast their ballots.
Catalonia has 7.5 million inhabitants and, accounting for roughly 20 per cent of Spain's economic output, is one of its wealthiest regions. It has a separate language, Catalan, a history of oppression from Madrid and grievances about subsidizing the rest of Spain.
Opinion polls have consistently suggested a lack of support for independence, though the Yes vote always expected to prevail, as unionists were seen as unlikely to take part in Sunday's unofficial vote.
The referendum was called September 6 by Catalonia's parliament and promptly invalidated by Spain's Constitutional Court.
It was Catalonia's second independence ballot in less than three years, with more than 80 per cent of 2.3 million voters backing a non-binding secessionist option in November 2014.
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About 90 per cent were in favour of independence, with about 8 per cent for the "no" camp and blank and void papers accounting for the rest.
Results will be forwarded "in the coming days" to the Catalan parliament "so that it may implement" a referendum law that obliges it to declare independence within 48 hours of a "yes" victory, Puigdemont said.
He also accused Spain of writing "a shameful page in its relations with Catalonia" and urged the European Union to hear out Catalan concerns.
"The European Union can no longer continue looking the other way," he said.
Some 844 people were hurt in clashes with police, according to Catalan health authorities, as officers in riot gear raided dozens of public buildings to prevent them from being used as polling stations.
Catalans had occupied the buildings before the weekend in a bid to keep them open.
"We had to do what we had to do," Spanish Prime Minister Mariano Rajoy said from Madrid. "Today there was no self-determination referendum in Catalonia," he said, and "democracy prevailed because the constitution was upheld."
Calling the referendum a "mockery of the very essence of democracy," Rajoy thanked judges, prosecutors and police, and claimed to have the full support of the EU and the international community, despite criticism from some politicians and high-profile figures.
Earlier, Puigdemont accused Spanish police of responding to "ballot boxes, ballot papers and schools" with "batons and rubber bullets." Such "police brutality will forever shame the Spanish state," he said.
Social media was filled with images of officers in tense stand-offs with crowds. Some people could be seen being dragged away by officers wearing helmets and carrying batons; others were injured and carried away in stretchers.
Spanish opposition leader Pedro Sanchez, of the socialist PSOE, said his country's territorial integrity "is at risk," while the radical left Podemos party and Barcelona Mayor Ada Colau called for Rajoy's resignation.
Rajoy said he would address parliament on Monday and summoned crisis talks between all parties represented in Madrid, including Catalan separatists. He said he would "never close any door" to dialogue, "but always within the bounds of the law and of democracy."
"Crowd control instruments" were used in only one of 70 raids, Interior Minister Juan Ignazio Zoido told broadcaster La Sexta. His ministry said on Twitter that 33 Spanish police officers were injured.
Zoido confirmed that the Catalan police, or Mossos d'Esquadra, asked "in writing" for Spanish counterparts to intervene in certain situations. The Mossos' willingness to carry out Madrid's anti-referendum orders had been in doubt.
Voting started at 9 am and ended on time at 8 pm (0700-1800 GMT). In one Barcelona school that served as a polling station, large crowds defended the building from the threat of police incursions, and as its gates were shut, people broke into the Catalan national anthem.
In the central Placa de Catalunya, where secessionists usually hold their rallies, the Yes camp set up a stage with four banners flagging up Catalonia's ambitions. They said: "Hello Republic, Hello World, Hello Europe, Hello New Country."
Catalan authorities prepared more than 2,300 polling stations. By 6 pm, Spanish police had managed to close only 319 of them, or less than 14 per cent of the total, Catalan government spokesman Jordi Turull said.
Voter registration was at times conducted manually as the Catalans' use of an online census was repeatedly sabotaged by Madrid. Long queues formed outside referendum sites, and some voters were moved to tears as they cast their ballots.
Catalonia has 7.5 million inhabitants and, accounting for roughly 20 per cent of Spain's economic output, is one of its wealthiest regions. It has a separate language, Catalan, a history of oppression from Madrid and grievances about subsidizing the rest of Spain.
Opinion polls have consistently suggested a lack of support for independence, though the Yes vote always expected to prevail, as unionists were seen as unlikely to take part in Sunday's unofficial vote.
The referendum was called September 6 by Catalonia's parliament and promptly invalidated by Spain's Constitutional Court.
It was Catalonia's second independence ballot in less than three years, with more than 80 per cent of 2.3 million voters backing a non-binding secessionist option in November 2014.
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