Yes, this song is my favorite, and I used it in the OP of a thread that I started about songs in movies: Favorite Movie Music
This song by Michel Legrand earned an Academy Award for Best Original Song in the mentioned 1968 movie. In the remake of the movie in 1999, starring Pierce Brosnan as Thomas Crown, Sting performed this song.
PS. Michel Legrand was first known for the theme song in the 1964 movie "The Umbrellas of Cherbourg" that also brought Catherine Deneuve to fame. Another well-known song of his is "The Summer Knows" in the 1971 movie "Summer of 42".