Terms of the deal with the right-hander, which was first reported by The Athletic, are unknown at this time.
Rondon, 29, spent his first five seasons with the Chicago Cubs, compiling an 18-13 record with 77 saves, 28 holds and a 3.22 ERA.
The former closer may best be remembered for his save in Game 4 of the 2015 National League Division Series against the St. Louis Cardinals.
The Cubs won the 2016 World Series over the Cleveland Indians, ending the team's 108-year drought.
On Thursday, the Astros introduced former Indians right-handed reliever Joe Smith after he signed with the team.
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