Seventy legislators voted in favour, 10 voted against, while two cast blank ballots.
The decision was made during a secret vote in Barcelona on Friday afternoon.
The names of those who voted for independence were withheld, as the Spanish attorney general promised to charge those who voted in favour of independence with “rebellion”.
After the declaration, the Spanish government said it will depose the Catalan President Carles Puigdemont and his cabinet, allowing Madrid to directly administer the breakaway region. The Spanish Prime Minister also announced the suspension of the top officials of Catalonia's regional police.
During the vote for independence, two right-wing parties, Citizens (Cs) and People's Party (PP), along with the centre-left Socialist Party of Catalonia (PSC), left the Catalan parliament before the vote in protest.
Alberto Rivera, president of Cs, took to Twitter to call the vote "illegal". Miguel Iceta of the PSC said it was a "spectacular error".
During the special plenary in the Catalan parliament on Friday, Carles Riera of the far-left Popular Unity Candidacy party asked that the declaration be voted upon.
"We take this step on our feet, with our heads held high. Not on our knees like subjects, but as free people without fear," he said.
'We must keep to our values'
As the votes were counted, thousands in Barcelona cheered as they gathered on the streets. After independence was declared, the demonstrators outside of the Catalan government palace called for the Spanish flag to be removed from the top of the 16th-century building.
Catalan President Carles Puigdemont called for calm ahead of an expected crackdown by Spanish authorities.
In front of a large crowd of fellow separatists, Puigdemont said: "In the days ahead we must keep to our values of pacificism and dignity. It’s in our, in your hands to build the republic."
"Catalonia is an integral part of Spain"
Reactions to the Catalan declaration have mostly called for dialogue to resolve the impending crisis. Donald Tusk, president of the European Council, said he hopes the government in Madrid doesn't result to force.
Charles Michel, prime minister of Belgium, echoed Tusk's call for dialogue and said it is the only way to resolve a political crisis.
To both reactions, Catalan President Carles Puigdemont replied that the Catalan government always favours dialogue.
In a reaction, the United States said it supports the Spanish government.
"Catalonia is an integral part of Spain, and the United States supports the Spanish government's constitutional measures to keep Spain strong and united," State Department spokeswoman Heather Nauert said.
Steffen Seibert, spokesman for the German government, said in a reaction that Germany does not support the Catalan declaration of independence.
He added that Berlin supported the "clear position" of Spanish Prime Minister Mariano Rajoy in his bid to restore calm and order.
In the UK, reactions were mixed.
UK Prime Minister Theresa May's office said Britain "does not and will not" recognise the Catalan regional parliament's declaration of independence, which "is based on a vote that was declared illegal by the Spanish courts".
But the Scottish government, led by the pro-independence Scottish National Party, criticised Spain for refusing dialogue and said imposition of direct rule by Madrid "cannot be the solution".
France's President Emmanuel Macron said he supports Spain's Prime MInister, saying "there is a rule of law in Spain with constitutional rules. Mariano Rajoy wants these rules to be respected and he has my full support."
Catalans voted in a disputed independence referendum on October 1 that was ruled illegal by the Spanish Constitutional Court and met with police violence, which was condemned by rights groups and European leaders.
The Catalan government said 90 percent voted for independence, but turnout was less than 50 percent.
Puigdemont announced independence on October 10, but suspended the declaration after eight seconds to encourage dialogue with Madrid.
No dialogue is known to have taken place.