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Mr Modi spent 90 minutes with 11 top CEOs including Eric Schmidt of Google, Ajay Banga of MasterCard and Indira Nooyi of PepsiCo.
He then met one-on-one with half a dozen CEOs. Describing his meeting with PM Modi as "excellent", General Electric chief executive Jeffrey Immelt said, "GE is a long-term investor in India. We look forward to more in the future."
"India is open-minded. We want change. Change that is not one-sided," Mr Modi reportedly said, according to a tweet by Foreign Ministry spokesperson Syed Akbaruddin.
He said the PM also told the CEOs that "Infrastructure development is a big opportunity".
After the breakfast meeting, Ajay Banga of MasterCard told NDTV that PM Modi highlighted two priorities - to generate jobs and improve the quality of lives of citizens.
Pitching for investment in infrastructure, Mr Modi told the business leaders that he would like to convert the recent cancellation of nearly 200 coal licenses by the Supreme Court into an opportunity to move ahead and "clean up the past".
The Supreme Court said the coal mining rights had been issued without transparency. The government will now be free to auction off the cancelled blocks by the end of this fiscal year.
Hours before he left for the US last week, Prime Minister Modi launched the ambitious "Make in India" campaign, guaranteeing that manufacturing in India will be made easy and cheap. He has earlier promised "red carpet and not red tape" for investors.
On Sunday, at a packed Madison Square Garden in New York, the Prime Minister repeated that promise and vowed to repeal archaic laws and make investing easier in the country.
The Prime Minister will also attend business meets in Washington on Tuesday during his second leg of the five-day visit. He carried gift packs of tea from India for the CEOs he met. Each box is signed by the Prime Minister.
(With inputs from PTI)