Originally cast in the lead roles were Sir Rex Harrison and Samantha Eggar, who were replaced by Richard Burton and Lee Remick. When MGM opted to replace Remick with Petula Clark, based on her reviews and Golden Globe nomination for Finian's Rainbow (1968), Burton balked at playing opposite a "singer" rather than an "actress", so Peter O'Toole was cast instead.
When the character of Ursula gushes over Mr. Chips, asking Katherine to let her have him when she was done with him, there is some truth in the line. Ursula, played by Siân Phillips, was, in real life, Mrs. O'Toole.
Siân Phillips wrote in her memoir that her husband Peter O'Toole was so well made up as the elderly Mr. Chips, that she walked past him in the canteen without recognizing him.
In her memoir "Public Places", Siân Phillips wrote that her husband Peter O'Toole refused to rehearse their scenes together.
Sherborne School, the filming location for most of the scenes set at Brookfield School, is an eminent British Public School. Amongst the school's former pupils is Alan Turing, who was played by Benedict Cumberbatch in The Imitation Game (2014), which also used the school as one of its filming locations. Other notable alumni of Sherborne School are writer John le Carré and actors Jeremy Irons and Hugh Bonneville.