On November 8, 1965, he was selected as the pilot for the planned Gemini 9 mission. Elliot See was nominated as his commander.
During the Gemini 6 and Gemini 7 flights in December 1965, he served as a liaison officer (Capcom) from the flight control center in Houston.
On February 28, 1966, the primary and backup crews of Gemini 9 flew to St. Louis in two T-38 Talon aircraft to visit McDonnell, the manufacturer of the Gemini spacecraft. Elliot See piloted the lead aircraft with Bassett as co-pilot. Due to poor visibility, See missed the runway at St. Louis Airport. After completing a low-altitude circuit, the aircraft clipped the roof of McDonnell Corp. Building 101 and crashed. See and Bassett were killed instantly. Building 101 housed, among other things, the spacecraft for the Gemini 9 and Gemini 10 missions.
Charles Bassett was buried in Arlington National Cemetery. His name is inscribed on the metal plaque of the Fallen Astronaut, the only artwork on the moon.

