Officers seized a van in north east Leeds and found 129,000 suspected illegal cigarettes hidden inside a fake compartment in the door of the vehicle.
The team from HM Revenue and Customs (HMRC) also found more than 11kg of hand-rolling tobacco, 35 litres of suspected illicit vodka and a further 9,000 cigarettes worth £51,159 in duty during the planned operation on Thursday, August 1.
The alcohol and tobacco were taken from two vans and three shops in the area - although the exact locations of the properties have not been identified.
The majority of the cigarettes were discovered when officers peeled back the door of a van, which was parked outside one of the shops where searches were carried out. The remaining cigarettes were found in another van outside a store managed by the same shop owner.
West Yorkshire Police and Trading Standards staff assisted HMRC with their enquiries.
'The illicit tobacco market costs the UK around £1.8 billion a year'
Eden Noblett, assistant director of the Fraud Investigation Service at HMRC, said: "The sale of illegal tobacco and alcohol will not be tolerated by us or our partner agencies.
"Disrupting criminal trade is at the heart of our strategy to clampdown on the illicit tobacco market, which costs the UK around £1.8 billion a year, and the sale of illicit alcohol which costs the UK around £0.9 billion per year. This is theft from the taxpayer and undermines legitimate traders.
"We encourage anyone with information about the illegal sale of tobacco or alcohol to report it online or call the Fraud Hotline on 0800 788 887."
The day of action was part of a wider police initiative aimed at tackling organised crime.
Detective superintendent Jaz Khan, of West Yorkshire Police, said: "A number of searches as part of multi-agency day of action resulted in what is clearly a very significant quantity of suspected illegal cigarettes and tobacco.
"The organisations who sell them can often be linked to organised crime. This is far from a victimless crime and we will continue to work with partners to pursue those responsible."
No arrests were made and enquiries are ongoing.
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