"Equally, there may be people who thankfully may have managed to escape the fire and for whatever reason have not let their family or friends or police know", he said.
"We are all desperately sad, we are angry, but of course none of us as angry as those who were directly affected".
Five people who had been reported missing after the disaster have been found safe and well, he added.
Police Commander Stuart Cundy gave the new figure during a statement outside Scotland Yard on Monday.
While emergency services have been widely praised for their handling of the disaster, the government has been criticised for a slow and inadequate response, with Prime Minister Theresa May facing public anger for failing to meet residents during her first visit to the site.
Cundy said the search and recovery operation was ongoing in the burnt-out 24-storey tower, which was built in 1974 and had received a major refurbishment that was completed past year.
They said: "We naturally welcome funds for those in need, though this does show once more the tendency to sideline residents' views".More news: Hearing scheduled on release of Cosby jury names - Western Mass News - WGGB/WSHM
Meanwhile, London mayor Sadiq Khan has said that high-rise tower blocks dating from the 1960s and 1970s could be torn down in the wake of the deadly fire.
"The awful reality of the fire that night means that we are supporting some people who may have lost a number of members of their family on that night", Cundy said. The measures were announced following the second meeting of the Grenfell Tower Recovery Taskforce, chaired by the Prime Minister.
The revised death toll comes as images showing the burned-out interior of the London tower block are released.
On the lack of sprinklers in Grenfell Tower, and other buildings, he said: "My understanding is that the best expert advice is that retrofitting sprinklers may not always be the best technical way of ensuring fire safety in a building".
If that death toll is confirmed, it would make the Grenfell Tower blaze the deadliest in London since World War Two.
Chancellor Philip Hammond said the cladding, which has been blamed for spreading the fire, is banned in Britain.
While he refused to speculate on the inquiry's outcome, Cundy said, "I would like to reassure everybody that we will be looking at all criminal offenses that may have been committed by any individual or organization".