It was not clear where Friday's groups were being taken, although one bus driver told TVE television he was taking his group to the airport.
An elderly couple could be seen leaving in an ambulance. But the authorities said there have been no new cases since the virus was detected in four Italian tourists earlier this week.
Half a dozen guests, including a baby in a pram, underwent temperature scans in the back of the hotel before boarding the first minibus, a video, shot by hotel guest Christopher Betts, showed. One of the people boarding said he was from Belgium.
Spain now needs to liaise with the governments of the remaining hundreds of guests, to establish monitoring protocols before they are allowed to return home, local health authorities confirmed on Friday.
"That is a more complicated process than it seems, because it involves several ministerial departments of their countries of origin", Fernando Simon, director of Spain's Centre of Coordination of Health Emergencies said.
A small group of guests who showed symptoms or who came into close contact with the infected Italians must complete the isolation period in their rooms, even though they have tested negative for the virus, Simon said.
They will be allowed to leave on March 10, local authorities added.
Inside the hotel, guests without symptoms were allowed to circulate freely, using the restaurants and swimming pools, as long as they wore protective masks, washed hands regularly and checked their temperature twice a day, according to instructions from the health authority.
Some guests complained that basic safety measures such as wearing masks and washing hands regularly were being ignored.
Spain's total number of coronavirus cases rose to 33 on Friday. The bulk of them were linked to Italy, the site of Europe's worst outbreak.
One of the cases involved a sports reporter from Valencia who had recently travelled to Milan, and the Valencia football club announced on Friday the suspension of all non-sports indoor events such as news conferences "that present risk to players, coaching staff and club staff".
The coronavirus can spread via droplets in the air when an infected person coughs, sneezes or breathes out, and these can also contaminate surfaces such as door handles and railings.
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