Almirola's Richard Petty Motorsports teammate Marcos Ambrose qualified second.
This is the first full season in the series for Almirola, and in his 47th career Sprint Cup start he turned in a lap of 192.940 mph. Ambrose was clocked at 191.598 mph.
Defending race champion Kevin Harvick qualified 14th. Danica Patrick, making her third Sprint Cup start, was awarded the 40th starting position on owner points after a poor qualifying lap of 185.179 mph.
The Coca-Cola 600 finishes off what is annually the biggest day of worldwide motor racing. The Formula One Monaco Grand Prix, the highlight event on that circuit, is also scheduled for Sunday, as is the Indianapolis 500.