I remember Jack Palance as Dr. Jekyll. That was around 1968-69. Made for TV movie. Not bad.
I have the Jack Palance version (The Strange Case of Dr Jekyll and Mr Hyde) as part of the Dan Curtis Macabre collection on DVD (also includes the 1973 Jack Palance film of Dracula, the 1974 version of The Turn of the Screw with Lynn Redgrave, and the 1973 version of The Picture of Dorian Gray with Shane Briant).