Barnet Council’s Trading Standards team seized more than £3 million in hand-rolling tobacco and other products during a series of raids across the borough.
The sting targeted five businesses and a self-storage container in Finchley, Colindale, Edgware, West Hendon and Golders Green.
Councillor Barry Rawlings, leader of Barnet Council and cabinet member for strategic partnerships, economy and effective council, said: “This work is important.
“Our Trading Standards Officers covertly inspect businesses on a regular basis to ensure they’re trading fairly and within the law.
“We take the health and wellbeing of our residents extremely seriously, and businesses should not be profiteering on the black market by selling products that will cause them harm.”
The investigation, known as Operation CeCe, led to the discovery of 3.6 tonnes of tobacco leaf packaged in 180 boxes.
Each box weighed 20kg and could have been turned into at least 72,000 pouches of hand-rolling tobacco.
The estimated street value was £3,121,200.
Officers also confiscated 4,506 cigarettes with a street value of £65,337, along with 309 pouches of hand-rolling tobacco, 973 vapes and 59.55kg of shisha tobacco.
Products were hidden behind secret doors, inside two vehicles, in a safe and in a large self-storage container.
The council was supported by the Met Police, HMRC and sniffer dogs Dora and Skye.
Just five days later, another operation led to further seizures targeting an alleged organised crime group.
The team busted a smoking store in Hendon and a linked shop in Tottenham.
They also targeted the Haringey and Ealing home addresses of two suspects.
Both individuals were taken into custody.
In this operation, officers seized 1,621 cigarettes, 2,435 vapes, 59 pouches of hand-rolling tobacco and more than £4,000 in cash.
Trading Standards and the police will be considering a full range of enforcement actions.
This includes, upon further investigation, the potential to prosecute, closure orders against problem premises and more.
It has warned businesses to buy products only from legitimate sources and keep printed invoices as proof.

