Besides Outalha, the probe agency also recorded the statement of a New York-based cousin of Headley through a questionnaire sent through the US Department of Justice, official sources said.
Headley, who is at present undergoing a prison term of 35 years in a Chicago jail for conspiring in terror attacks in Mumbai and Denmark, had started a video parlour in New York in 1997.
The legal process of quizzing Outalha concluded only after the NIA sent a fresh request in French to Moroccan authorities for recording her statement pertaining to her knowledge of her estranged husband's association with LeT terror group. French is generally used by the Moroccan government for international diplomatic communications.
The NIA had registered a case in 2009 to probe the activities of Headley in India.
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In the absence of any Mutual Assistance Legal Treaty between India and Morocco, the LR had been issued on the basis of "Assurance of Reciprocity", thereby promising the African country of all assistance in any legal cases in future.
Outalha had visited India twice and was used by Headley, a US national whose father was a Pakistani and mother a white American, while carrying out a reconnaissance mission at Hotel Taj Mahal in Mumbai.
The NIA, however, refused to share information tendered by Outalha.
Earlier, Headley's another wife Shazia and business associate Raymond Sanders had turned down a similar request of NIA to answer questions related to his association with the terror group, citing a US privacy law.