Officials said the agency arrested Reddy, K Sreenivasulu and Prem Kumar yesterday under provisions of the Prevention of Money Laundering Act (PMLA) after they were called for questioning at the Enforcement Directorate (ED) office here.
The agency said it has "reasonable belief that these three persons are involved in money laundering."
The three were later produced in a court which sent them to jail till March 28. They are now lodged in the Puzhal central jail, they added.
A total of five people have now been arrested in this case by the ED as it had earlier nabbed Mahavir Hirani and Ashok Jain in December last year.
The agency had filed a criminal complaint against Reddy and others based on a CBI FIR in the case which was registered after the I-T department first searched his and his associates' premises in November, 2016.
The ED in a statement said Reddy told it that "cash seized by the Income Tax department belongs to his SRS mining company and he admitted that it was unaccounted money.
The I-T department has made one of the biggest detection of alleged unaccounted income of over Rs 142 crore in this case with the seizure of Rs 34 crore in new notes, post demonetisation.
The Reddy case and the other involving Delhi-based lawyer Rohit Tandon and Kolkata-based businessman Paras Mal Lodha are being probed by at least four agencies-- the ED, the Income Tax department, the CBI and Delhi Police, and are considered the most high-profile black money cases being investigated in the aftermath of the notes ban.
"He (Kumar) stated he used to receive demonetised currencies for procuring gold bars through Srinivasulu, an associate of Reddy. He also stated that the seized 30 kgs of gold bars in his premises also belong to Reddy only.
"Srinivasulu has stated that he used to receive money from SRS mining and used to use a part of the same for converting into gold bars through Prem Kumar as per the instructions of Reddy. Remaining cash was kept at various premises and the same was earlier recovered and seized by the I-T department," it said.
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