The astronaut will become chief operating officer of the Montreal Science Centre, a federal museum with a variety of interactive exhibits and educational movies.
The two-time space traveller will begin her new job July 15. She also becomes vice-president of the Canada Lands Company, which hosts the site at Montreal's Old Port.
"In a modern and innovative society, where advancements are plentiful and communication is instantaneous, science and technology are a part of everyday life," Payette said in a statement Wednesday.
"Science is fun, and it's fundamental."
Payette has most recently been a Quebec government scientific envoy to Washington, D.C.
Her appointment will douse speculation that she might take over the Canadian Space Agency, which is currently looking for a new president.
An engineer and researcher before she was recruited to the space agency, Payette made trips to space in 1999 and 2009.