Just 7.83% of voters opted to remain part of Spain in Sunday’s poll.
Regional government sources have claimed Catalonia will declare its independence from Spain as early as Monday.
With the overwhelming pro-independence result confirmed, pro-independence politicians in the Catalan parliament are planning a debate and vote on the matter as their first order of business for next week.
The official declaration of independence is expected to follow shortly after.
Catalonia’s regional government leader Carles Puigdemont says he already feels like the “president of a free country” after the controversial poll.
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He told German newspaper Bild: “I already feel as president of a free country where millions of people have made an important decision.”
The independence referendum was marred by a violent police response as officers attempted to shut down polling stations.
The Spanish government claims the referendum is illegal and should not have taken place, as Catalan officials failed to follow constitutional processes when the vote was called.
But the authorities’ handling of the referendum has been heavily condemned after images of violent police clashes emerged.
Dr Ramon Pardo, a senior lecturer in international relations at King’s College London, told Express.co.uk: “I think the most important question is how is [Puigdemont] going to word the declaration [of independence].
“That is probably going to be more crucial than the declaration itself.
“If he says ‘as of tomorrow Catalonia will be an independent state’, this will be seen as very confrontational to the Spanish government.
“If he says ‘we are going to start a constitutional process that will lead to independence’, that is a more conciliatory tone because he is leaving the door open to negotiations.”
Either way, the declaration will not be valid under Spanish law, Dr Pardo explained.