The weekly cabinet meeting usually takes place in Madrid but Prime Minister Pedro Sanchez's Socialist government decided to hold it in the Catalan capital, igniting protests.
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Brussels police said that around 45,000 people attended the rally, which comes just two weeks ahead of regional elections in Catalonia.
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Ousted Catalan president Carles Puigdemont says he will stay put in Brussels as Spain’s top court ordered the suspension of the Catalan parliament’s independence declaration.
Catalonia's deposed separatist leader Carles Puigdemont said his region's independence drive should "slow down" to avoid unrest as Madrid imposes direct rule on Catalonia.
The session is in response to the Spanish government invoking Article 155 of the Spanish constitution allowing the central government to intervene in running Catalonia, after the region voted in favour of independence in a banned October referendum.
The elections will be held in January. Spain is set to impose direct rule on Catalonia as its leader has refused to back down from his independence plan.
The Spanish government said in a statement they will invoke article 155 of the constitution. Catalonia's regional government had earlier said in a letter that independence will be declared if Spain offers no talks.
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