A protest led by relatives of the politicians and activists arrested and being held in jail for organising the Catalonian independence referendum on 1 October, saw a crowd of around 750,000 filling more than 3 kilometres of the Carrer de la Marina in Barcelona.
The demands included safe passage for Carles Puigdemont and former cabinet members in exile in Brussels. All have been charged with sedition and rebellion, and face a maximum 30 years in jail, if found guilty.
Puigdemont and his colleagues in Belgium sent messages of support to those struggling for the liberation of the prisoners.
Puigdemont also published a video appeal, "to send a very clear message: to the Spanish State, that this can not continue; to the European Union, to stop looking the other way. And to all the Democrats in the world, we say that these people stand with dignity and there are no prison bars or exiles that can dissuade you from doing what is allowed for democrats in the world: to decide your future at the polls."
Several hundred people turned up for a rally in Brussels on Sunday, also in support of the Catalonian independence, to criticise the EU and to demand that the Spanish government releases the jailed regional officials.
Last Wednesday, a strike called by a pro-independence union caused travel chaos, blocking roads and train lines including Spain's main link to France and the rest of Europe.
"Democracy in Spain is not only sick, it is practically dead," the Spanish MEP, Josep-Maria Terricabras, said to the protesters backing Catalan independence.
"I think that it is absolutely terrible that the European institutions don't understand that when you attack democracy you cannot applaud Rajoy and those institutions in Spain that are outside the law," added Terricabras.
The Brussels protest was outside the European Union's main building and followed Saturday’s demonstration in Barcelona.
Flags from Belgium's Dutch-speaking region of Flanders were waved at the protest as there is sympathy for the Catalonian cause among Flemish nationalists.
The EU was "founded to not see the return of dictatorship and fascism in Europe," ousted Catalan Minister of Health, Antoni Comin, said to the crowd which interrupted with chants of "Libertad!" and "Not all here" in reference to the jailed officials.
Comin is one of five officials who fled to Belgium after Spain dismissed the Catalan government and imposed direct rule on the semi-autonomous region following the declaration of independence by Catalonia’s parliament in October.
Spanish PM, Mariano Rajoy, visited Barcelona on Sunday and performed a U-turn by urging businesses not to abandon Catalonia. This was after hundreds of companies moved their legal headquarters away as the uncertainty over the region continues.
These relocations were speeded by Rajoy's government successfully passing new laws to enable a smooth transfer of head offices from Catalonia to other of Spain’s regions, a move that 2,400 companies already have made due to the instability of the region and its unclear political future.
“We have to recover the sensible, practical, enterprising and dynamic Catalonia... that has contributed so much to the progress of Spain and Europe," Rajoy told an assembly of 1,000 members of his Popular Party in Barcelona, adding that he had “exhausted all roads” after the Catalan government’s unilateral declaration of independence and called on the participation of the “silent majority” to “convert their voice into a vote”.
“We will never let anyone break the ties that bind us," said the Spanish PM, “We must recover Catalonia from the havoc of separatism.”
Rajoy did not make a public appearance in Barcelona, restricting his comments to the party faithful.