Fuel subsidies are a massive expense in India, contributing to an overall subsidy bill that ballooned to $43 billion, or two percent of gross domestic product (GDP), under the previous government.
"I appeal to all those who can afford cooking gas at market rates to please give up your gas subsidies," Modi said at an energy conference in New Delhi.
"The money we save with your help, we will use for the poor so that they have access to clean energy too."
He said 280,000 consumers had already voluntarily unsubscribed from a programme that offers subsidised cooking gas, helping the government save $16 million.
Many poor Indian households cook their meals over smoky earthen stoves fired by wood, hay or cow dung, causing respiratory problems - particularly among children.
The Indian leader also said the country should cut oil, gas and petrol imports by 10 percent over the next seven years as it seeks to reduce its energy bills and become more self-sufficient.
Since taking office last year, Modi has lifted diesel price controls to reduce the national energy bill and opened millions of bank accounts to enable subsidies to go directly to the poor and circumvent corruption.
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