Tens of thousands have protested in Madrid, while other demonstrations have been held in the Catalan city of Barcelona urging political dialogue.
Campaigners gathered with signs saying "Spain is better than its leaders" and "let's talk".
Businesses have continued to announce their departure from the Catalan region amid the ongoing political uncertainty.
The Caixa Foundation, which controls one of the Spain's largest banks, announced it was moving its headquarters to Palma de Mallorca while the crisis continues.
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