Six shops were raided and contraband, including tobacco and shisha, was found with help from detection dogs Skye and Fred.
One vehicle used to store illegal goods was seized and will be destroyed if not claimed.
The council says the action is part of a zero-tolerance approach to illegal tobacco linked to organised crime.
Alongside raids on six shops, officers identified vehicles being used to store contraband.
One of the vehicles linked to the investigation was seized and removed by the Council. It will be destroyed within 28 days if not claimed.
Jason Perry, Executive Mayor of Croydon, said: “Illicit tobacco sales are not a victimless crime. They are often linked to organised crime and are a blight on Croydon’s residents and genuine businesses.
“This operation demonstrates our zero-tolerance approach to those who profit from criminal activity at the expense of our communities. If you are selling illegal tobacco in Croydon, we will take action.
“I would also encourage residents to report concerns about illicit tobacco sales so that we can continue to protect local businesses and keep our neighbourhoods safe.”
