The two day operation began yesterday and has so far seen officers visit 2,525 London venues.
Police have targeted shops, supermarkets, pubs and clubs as part of the initiative, as well as minicab drivers and betting shops.
Scotland Yard has described the crackdown, which is codenamed Operation Condor and involves 1,500 officers from across all 32 boroughs, as one of the biggest policing operations of the year so far.
A total of 133 people were arrested yesterday with officers reporting or disclosing 327 offences.
Around 1,000 counterfeit cigarettes, 50 litres of counterfeit vodka, 300 packs of chewing tobacco and 250 cases of alcohol was also seized.
It comes after a similar operation in February that saw 4,896 licensed premises visited over a period of 48 hours.
A total of 658 licensing breaches were identified with police making 420 arrests.
Commander Mak Chishty, who is leading the operation, said: "Operation Condor is back again and will continue to target those who flout licensing laws.
"We want to ensure that alcohol in our pubs and clubs is sold and consumed in a responsible way and on our roads vehicles, such as taxis are properly licensed and safe."
He added: "The results of unlicensed activity on our streets can find the form of underage drinkers acting unsociably close to where we live, unlicensed mini-cabs endangering passengers by making uninsured journeys and also shops who potentially encourage the circulation of stolen items by not correctly checking the history of second hand goods offered for sale."
The Mayor of London, Boris Johnson, said: "Whether it's unlicensed minicabs which endanger women, the illegal sale of alcohol or the selling of weapons to our young people, this immoral behaviour contributes to serious crime across London.
"That is why operations like this by the Met are so important and I hope this crackdown will be every bit as successful as past efforts."