They are hunting for Moroccan-born Younes Abouyaaqoub, now named by Spanish media as the suspected driver.
A man previously reported as the key suspect, Moussa Oukabir, 17, was one of five men killed by police after a later attack in Cambrils, west of Barcelona.
Police say the suspects had been planning more sophisticated attacks.
They said blasts on Wednesday at a house in the town of Alcanar deprived plotters of bomb material, so they carried out simpler attacks using vehicles.
Abouyaaqoub, 22, lived in the town of Ripoll to the north of Barcelona. Three people have been arrested in Ripoll and one person in Alcanar.
Oukabir had previously been seen as the central figure, but police now think that Abouyaaqoub is the main suspect.
Oukabir is suspected of using his brother's documents to rent the van used in the Barcelona attack and another found hours later in the town of Vic, north of Barcelona, that was intended as a getaway vehicle.
Another van, a Renault Kangoo, is also being sought, amid reports it may have been driven across the border into France.
In the early hours of Friday police shot dead five attackers, including Oukabir, in Cambrils after the men drove a car into pedestrians, killing one woman and injuring six other people.
The attackers' vehicle overturned and when the men got out they were quickly fired upon by police. One of the attackers was reportedly brandishing a knife.
The men were wearing what appeared to be explosive belts but these proved to be fake
Officials believe a cell of at least a dozen people was operating at the Alcanar house, which was being used as a bomb factory to prepare more devastating attacks than those in Barcelona and Cambrils.
Interior Minister Juan Ignacio Zoido said on Saturday that the cell had been "totally dismantled", but that security measures around the country were being increased, particularly in tourist areas.
However, the Catalan regional government suggested several more suspects were still at large.
Special police controls are being introduced at Saturday's two La Liga football matches in Barcelona and Girona.
The nation's security alert level is staying unchanged as there is no information suggesting an imminent attack.
Only five of the dead have been named so far:
A 74-year-old Portuguese woman, a 40-year-old woman with dual Argentine and Spanish citizenship, and a Belgian were also killed, their governments said.
The whereabouts of seven-year-old Julian Cadman, a dual British-Australian national apparently separated from his injured mother during the attack, remains unclear. He was widely reported to be missing.
However, the Catalan police, responding to inquiries, tweeted that they had neither been looking for nor found any missing child. The victims and the injured had all been located, they said.
Catalan emergency services gave a new breakdown of the injured on Saturday:
Pegged on strings between the lamp-posts and plane trees on the packed boulevard, more and more sheets of white paper flap in the breeze.
Imprinted with a red love heart, each contains a message left by a stroller, reflecting on the attack. Messages of love for Barcelona abound but there is anger too. "Now we need to take action," reads one. "I don't want to run any more. Let's not run away from them, let's run after them."
The Mellouli family's message, in French, says: "Sousse (Tunisia) supports Barcelona against terrorism". Sousse, the holiday resort where a gunman killed 38 people just over two years ago, now shares sorrow with Barcelona.
"We are very upset by what happened here," says the father, Slah, who is here on holiday with his family. "We are all against terrorism. Islam is against terrorism too. What happened here is not Islam. Nobody can be safe from terrorism now and we must unite against it."
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Barcelona attack: New manhunt for suspected driver
The driver in Thursday's van attack that killed 13 people in a tourist area of Barcelona may still be alive and on the run, Spanish police say.