He asked the region's government to give up its "escalation of radicalism and disobedience".
The Spanish authorities have sought to stop the vote, which they regard as illegal, by seizing voting materials. Police searches in the Catalan capital, Barcelona, sparked a mass street protest on Wednesday.
An estimated 40,000 people blocked the entrance to the Catalan economy ministry late into the night. Separatist parties who control the Catalan parliament pushed through the referendum law earlier this month after unsuccessfully demanding for years the right to hold a free vote on self-determination.
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