Fresh arrests have been made in the investigation into the London Bridge attack, including two men who were held in a swoop by armed officers.
Counter-terror police arrested the pair during an operation on a street in Ilford, east London, Scotland Yard said.
One of the men, aged 27, was held on suspicion of the preparation of terrorist acts, while a 33-year-old was arrested on suspicion of possession with intent to supply controlled drugs.
A third man, aged 29, was arrested on suspicion of the preparation of terrorist acts at an address in Ilford during the operations late on Wednesday night.
All three men have been taken into custody for questioning at a south London police station while detectives search the residential address and a business premises in Ilford.
The arrests follow the detention on a 30-year-old man as detectives raided an address in Ilford in the early hours of Wednesday.
A Scotland Yard spokesman said: "Detectives investigating the London Bridge terror attack have made three more arrests and carried out two more search warrants in east London late on Wednesday June 7.
"From around 10pm, officers from the Met's Counter Terrorism Command, supported by firearms officers, arrested two men on a street in Ilford, a third was arrested after a warrant was carried out at a residential address in Ilford."
The developments came as families of the London Bridge attackers expressed their disgust at the murderous rampage which left eight people dead on Saturday.
Both the relatives of Khuram Butt and the ex-partner of Rachid Redouane distanced themselves from the extremists, saying the atrocity had left them shocked.
Their condemnation came as footage emerged online appearing to show the moment armed police gunned down the three knife-wielding terrorists.
In the CCTV, the trio can be seen rushing at a passing pedestrian near Borough Market, raining down a series of blows while police cars approach.
The marksmen are charged as they train their guns on the attackers, with one knifeman, who appears to be Butt, swinging his weapon wildly towards an officer.
A volley of gunfire in unleashed during the melee and all three perpetrators are felled within seconds, the footage shows, eight minutes after the emergency services were first called.
During the confrontation, brave passers-by can be seen throwing missiles in the direction of the gang and their last victim is shown stumbling away at the end of the clip.
Separate video published by The Times shows the conspirators meeting in the dead of night on May 29, five days before the attack.
According to the paper, the images were captured near Butt's gym, the Ummah Fitness Centre in Ilford, east London, and show Redouane placing his phone on the floor, before the men move down the road for 10 minutes.
Butt wore an Arsenal shirt and a fake suicide belt during his bloody spree and was later pictured sprawled on the concrete outside the Wheatsheaf pub.
On Wednesday, the 27-year-old's family said they were "shocked and appalled" by his actions.
In a statement, they wrote: "As a family we are shocked and appalled by the actions of Khuram and his associates.
"We strongly condemn these actions.
"Our heartfelt thoughts and prayers are with the victims and families at this time.
"Now more than ever we need to work together to stop the actions of the mindless few who claim to be acting in the name of Islam."
As the fallout from the atrocity continued, all eight people killed in the massacre were identified, while a further 10 victims remain in a critical condition.
The ex-partner of 30-year-old Redouane earlier spoke of her shock at discovering he had inflicted the outrage on the capital.
Charisse O'Leary said she has "shed many tears for the people caught up in this horrific incident".
In a statement released to the Press Association, she said her "heartfelt thoughts go out to all those murdered or injured" in the events of Saturday night.
"I am deeply shocked, saddened and numbed by the actions of my ex-partner who has killed and injured so many innocent people," Miss O'Leary said.
She said she had been separated from Redouane for six months.
"We have a beautiful young daughter, that for the last six months has been our only bond and reason for contact," she continued.
"My thoughts and efforts now are with trying to bring up my daughter with the knowledge that some day I will have to try and explain to her why her father did what he did.
"I wish to make it absolutely clear, so there can be no doubt, I condemn his actions and do not support the beliefs he held that led to him committing this atrocity."
Meanwhile, controversy over the UK's counter-terror efforts spread to border security after claims emerged that another of the perpetrators was let into the country despite being on a security watch list.
Youssef Zaghba is said to have been stopped by Italian officers trying to travel to Syria last year and added to an international database of alerts about individuals, to which the UK has access.
Questions over the extent to which the terror gang were known to security services have been mounting since it was revealed Butt had been investigated in 2015.
An al Qaida recruiter turned FBI informant, Jesse Morton, told The New York Times he reported to US authorities that Butt "had expanded his influence" in al Muhajiroun, a banned terror group in the UK, in 2015.
He had interacted with the future mass murderer on an extremist chatroom.
"My handler got back to me and said it was 'excellent work' and forwarded it to the head office," he told the paper.
The revelations add to concerns that security services repeatedly missed opportunities to stifle the threat from Butt, who was also reported for extremism in Britain and appeared in a Channel 4 documentary about jihadists.
Police have said Redouane was not known to authorities.
With cordons lifted around the site of the atrocity, Transport for London were forced to apologise after traffic wardens issued parking tickets to cars trapped in the crime scene since Saturday night.