This is one of two collaborations on Love and War with hip-hop producer Timbaland. Paisley told Billboard magazine: "His instinct was that making hip-hop would be wrong in every way for me. So where do we gel best? He said, 'Country and hip-hop come together in bluegrass,' since it's all about the rhythm. So in the studio, Timbaland's beating on a banjo with a pair of brushes, and it sounds like a jug band. That's what led to 'Grey Goose Chase.'"

It was the song's co-writer Canadiam musician Jared Gutstadt, who hooked up Paisley with Timbaland. The country star explained: "There's a great guy named Jared who we co-wrote these songs ["Grey Goose Chase" and "Solar Power Girl"] with, who is also a writer and a friend of mine. It was his idea to get together. He had been working with Tim and he said that the three of us would be an interesting thing to see what would happen."

The song's title references Grey Goose, a luxury vodka that was first developed in France for the American marketplace in the mid-1990s.