More than 500 cars have been seized and 66 people arrested so far in an operation targeting uninsured drivers in London.
The day-long operation, overseen by the Metropolitan Police Commissioner Bernard Hogan-Howe, is also designed to disrupt other criminal activity.
Up to 80% of uninsured drivers were involved in other crimes, he said.
Incidents of uninsured driving on Merseyside fell by 40% after Mr Hogan-Howe used the measure there.
"[Uninsured drivers] are also more likely to be involved in crashes and have unsafe cars, so we're taking this action to make London's roads safer," the commissioner added.
"This is the first of the operations I have asked for where officers across the Met will spend a dedicated day on a regular basis targeting uninsured drivers and those believed to be connected to crime."
The arrests were made for crimes including possessing drugs or an offensive weapon, driving whilst disqualified and driving while wanted on an arrest warrant.
The operation, which involved 1,000 officers, also led to a stolen lorry being stopped in Horseferry Road, Westminster, central London, a few minutes after it was reported stolen.
Cannabis, a large bundle of cash and a lock knife were found when a car was searched in Harleyford Road, Kennington, south London.
Roadside checkpoints using automatic number plate recognition have been deployed.
Uninsured vehicles have been impounded and could be destroyed, while offenders will be prosecuted.
The penalty for driving a vehicle without insurance is six penalty points and a £200 fine and can lead to a driving ban.
According to the Motors Insurers' Bureau, uninsured drivers increase other motorists' annual insurance premiums by £30.
They are also said to be five times more likely to be involved in road collisions.
In 2010 Scotland Yard seized 34,000 vehicles and prosecuted thousands of people who had no car insurance.
Jenny Jones, a Green Party Assembly Member who has campaigned on the issue, said: "It's great to see the new Met Commissioner taking a direct approach to tackle the problem of illegal drivers.
"I want the commissioner to stick to his suggestion that London should be doing exactly what he achieved in Merseyside.
"We need to take nearly three times as many vehicles off the road as we do now."
She added: "If we really want to crack down on the problem, we're going to have to take almost 100,000 illegal vehicles off the road each year."