"My thoughts are with the victims of today's terrible attack in Barcelona and the emergency services responding to this ongoing incident. The UK stands with Spain against terror," she wrote on Twitter.
At least 13 people died and more than 50 others were were injured when a van was driven into pedestrians on Barcelona's Las Ramblas boulevard, regional interior minister Joaquim Forn said.
British Foreign Secretary Boris Johnson said he was "concerned and saddened" by the attack on Las Ramblas, a busy shopping street popular with tourists.
Britain has suffered a series of terror attacks in recent months, with a suicide bomber killing 22 people at a concert venue in the city of Manchester.
Three attacks in London have all involved vehicles being driven into pedestrians, two of which saw assailants attack people with knives in the immediate aftermath.
London Mayor Sadiq Khan said the British capital "stands with Barcelona against the evil of terrorism".
"My thoughts are with the victims of this barbaric terrorist attack in the great city of Barcelona and with their brave emergency services," he tweeted.
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