A number of the pedicabs, described as "death traps" by Westminster City Council, have been seized in the operation on Thursday evening.
Police said about 80% of London's 1,000 pedicabs have been illegally adapted to run partially on car batteries, allowing them to reach speeds of 20mph.
Many of the drivers are uninsured and some flout traffic laws, officers said.
Last month bystanders narrowly avoided injury after a pedicab mounted the pavement in central London's Soho and smashed into a restaurant window.
In a crackdown on illegal rickshaws, council officials, along with officers from City of Westminster Police and Traffic Unit, set up a series of checkpoints in the West End and seized the electrically assisted pedicabs.
Councillor Danny Chalkley said: "The sheer number of these death traps has left us with little choice other than to take firm action.
"At the moment what should be a fun visit to the West End could all too easily turn into a tragedy for innocent passengers, and I'm not prepared to stand by and wait for that to happen."
Responsible pedicab operators have supported the crackdown which coincides with the council's proposals to install the first-ever designated pedicab bays in London for operators who abide by a code of conduct.
The voluntary code requires all drivers to be insured, undergo training and to have bikes regularly serviced and kept roadworthy.
Graeme Rivett, from London Pedicabs, said: "I am shocked at how in such a short space of time so many cowboy pedicab operators have come on to the streets, and they don't give a damn for the safety of anybody.
"It's a miracle nobody has been seriously injured or killed."
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