A German woman who was in a critical condition in hospital has died, as a direct result of the injuries she suffered in Barcelona.
Hours later, a auto sped into Cambrils, about 75 miles (120km) south of the city, hitting people before crashing into a police vehicle.
A cell of 12 jihadists has been blamed for the attacks.
The five occupants of the Audi A3 then jumped out and went on a stabbing spree, killing a woman before being shot dead by police. Another man was stabbed to death in a carjacking as the van driver made his getaway.
After the death of the driver of the van that wound up hundreds of passers-by in that Barcelona artery, the Mossos disintegrated the criminal command, although they are still investigating possible global connections of its 12 members.
The campaign will remain stopped, however, until after a large anti-terrorism show of unity demonstration set to take place on Saturday afternoon, where leaders of all the main Spanish and Catalan political parties are expected, along with tens of thousands of people.
The march was led by emergency workers, store keepers and residents of the city's Las Ramblas Boulevard.
About 500,000 people marched along the streets in a defiant act of solidarity and peace on Saturday (local time).
Prime Minister Mariano Rajoy said Friday the investigation into the attacks will be coordinated from now on by the Interior Ministry's organized crime and terrorism intelligence center, CITCO, after representatives of intelligence agencies and police forces met Thursday with judicial authorities at the country's National Court, which handles terrorism cases.
Following a week dominated by the response to the deadly attacks in and near Barcelona, Colau told reporters she wanted the "streets of Barcelona to be overflown by people".