Ambani, 64, deposed at the office of the federal agency in south Mumbai.
Ambani's statement was recorded as part of a fresh case filed under various sections of the Foreign Exchange Management Act (FEMA), the sources said without elaborating.
The industrialist had appeared before the ED in 2020 in a money laundering case against Yes Bank promoter Rana Kapoor and others.
In August last year, the income-tax department issued a notice to Ambani under the anti-black money law for allegedly evading Rs 420 crore in taxes on undisclosed funds of more than Rs 814 crore held in two Swiss bank accounts.
The Bombay High Court, in March, ordered an interim stay on this I-T show-cause notice and penalty demand.