The agency conducted the searches on July 1 at 10 locations in the national capital including at Pitampura, Vikaspuri, Rohini and Wazirpur of Naresh Chand Jain, whom the ED identified as a 'hawala king'.
It said details of some foreign bank accounts were also seized during the operation.
"The searches were conducted on the basis of information received by the directorate (ED) that Naresh Chand Jain and his brother Bimal Kumar Jain are involved in large scale hawala and illegal activities.
The seized Rs 27 lakh includes Indian and foreign currencies from Dubai, Hong Kong, the US and the Philippines.
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Documents related to various shell companies, stamps, letter heads, fake/bogus invoices of various shell companies were also recovered apart from hard discs, mobiles, several Permanent Account Number (PAN) cards, voter ID cards, digital payment devices of various foreign banks and SIM cards of Nepal and Dubai, it said.
The ED said Naresh Chand Jain and his brother have been "doing" hawala transfers to Dubai, Singapore, Hong Kong, China, Nepal, the United States of America, Europe and other countries.
The ED said its investigations have found that Naresh Chand Jain "registered shell companies by paying certain persons a sum of Rs 5,000-50,000 for becoming a director in his companies.
"These fake directors and shell companies were later used by Naresh Chand Jain and his associates for hawala and illegal activities," it said.
A hawala transaction pertains to movement of funds by the illegal usage of banking channels and others.
The agency is investigating the case under sections of the Foreign Exchange Management Act (FEMA) even as it is looking at possible money laundering instances in the case.