A senior official said 10 teams of 250 I-T sleuths swooped down on the official and residential premises of the group in Chennai and Puducherry early today.
Apart from the cash seizure, voluminous documents regarding collection of students fee, capitation funds and others were also recovered, he said.
"About Rs 80 crore has been seized since the operation that began early morning today. Apart from documents, a number of computer hardware have also been seized. This is one of the largest cash seizures in one operation in the country," the official said.
He said the operation was carried out based on inputs that the institution was allegedly trying to charge more money than the stipulated amount under the capitation and donations front, despite enjoying IT exemptions for being an educational institution.
Sources added that the department has also recorded the statements of various officials of the institution and the operation is expected to continue till tomorrow.