The online activist network announced it was launching “Operation Catalonia” after taking down a number of state-owned websites in recent weeks.
The latest cyber attack took place on Tuesday night, when the Royal House website was taken down by hacktivists.
That follows the website of the Constitutional Court – which ruled Catalonia’s October 1 referendum illegal – crashing due to an Anonymous-led DoS attack.
The website for the Ministry of Public Works and Transport was also hacked to display a “Free Catalonia” banner.
A number of Twitter accounts claiming to be part of the Anonymous network have warned of future attacks on Spanish government websites, which has been criticised for its violent response to the ballot.
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According to another Anonymous account, the Spanish police, who were filmed brutally attacking Catalans with batons and pepper spray, will be attacked shortly.
Anonymous had previously stated its support fro the Catalonian referendum in a video posted on YouTube shortly before the vote took place.
A hacker, in trademark Guy Fawkes mask and newsreader pose, said: “We wish to state that the Catalan people’s desire to express their will via a referendum is the majority view and cuts across all strata of society.”
Spain has become engulfed in a constitutional crisis following this month’s vote, in which 90 per cent of the 2.3 million Catalans who made it to the ballot box voted for independence.
Madrid has refused to recognise the vote, and the Constitutional Court ruled it illegal on October 17.
Spanish Prime Minister Mariano Rajoy has threatened to implement Article 155 and seize control of the semi-autonomous region.
Mr Rajoy’s administration had indicated that it was prepared to consider stopping the imposition of Article 155 if Catalonia called a snap election.
But today Catalonia leader Carles Puigdemont ruled out an election, to the upset of hard line separatists.