The raid on the home of Otoniel Usuba was part of a massive police operation in seven cities in Antioquia state in which 22 people were arrested, Colombia Reports said Monday.
Usuba, who has not been arrested, is the only surviving brother of the family that ran the organization.
The money, which was found in buried milk cans, was reportedly made from drug trafficking, illegal mining and the sale of land stolen from local farmers.
More than $1 million was also found hidden in furniture in apartments in Medellin.
Among those arrested was Usuba's sister, Nini Johan Usuga. Police said she stashed money in her brother's properties that was used to pay other criminal organizations.
Usuba's cousin, Alrey Usaga, also was arrested. Police said he oversaw drug trafficking in Central America.
During the five-week operation, police said they destroyed seven clandestine runways and left two airplanes and 37 speedboats inoperable. Seven backhoes used in illegal mining operations were seized.