As tensions continue to run high, independence supporters are set to rally in Barcelona at 1500 GMT calling for the release of Jordi Cuixart and Jordi Sanchez, the leaders of two powerful grassroots separatist groups who have been in jail since Monday pending investigation into sedition charges.
Autonomy is a highly sensitive issue in Catalonia, which saw its powers taken away under the dictatorship of General Francisco Franco.
During the meeting, which started around 10:00 am (0800 GMT), Prime Minister Mariano Rajoy and his ministers will decide on what powers to take away from the wealthy region, which now enjoys wide autonomy including control over its own policing, education and healthcare.
The Spanish government moved to activate a previously untapped constitutional article Saturday so it can take control of Catalonia.
The drastic escalation of Spain's worst political crisis in decades will see separatist leader Carles Puigdemont and his administration stripped of their jobs, Prime Minister Mariano Rajoy told reporters after a crisis meeting of his cabinet.
"We are applying Article 155 because the government of a democratic country can not accept that the law is ignored".
It's never been used since the 1978 Constitution was adopted, but Rajoy's conservative government says establishing direct control over Catalonia was a move of last resort.
"And at the same time we need to return to institutional normality".
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In Spanish, he accused Madrid of "attacking democracy".
King Felipe vowed: 'Spain will deal with this unacceptable attempt at secession by using the constitution'.
The vote itself was marred by sporadic violence as police took action to shut down some polling locations.
Though she opposes the independence drive, Barcelona mayor Ada Colau also deplored Madrid's decision, tweeting: 'Rajoy has suspended the self-government of Catalonia for which so many people fought.
Oriol Bartomeus, politics professor at the Autonomous University of Barcelona, said the central government was taking a huge risk.
Mr Rajoy was notably scant on details and long on justification for direct rule in his speech, essentially limiting his much-anticipated package of specific measures to a broad-brushed description of the whys and wherefores for his government's substitution of the nationalist ministers.
"I ask the parliament to meet in a plenary session during which we, the representatives of the citizens' sovereignty, will be able to decide over this attempt to liquidate our government and our democracy and act in outcome", Puigdemont said in a televised speech.