I know I've mentioned this series before but I'd go with Boris Karloff's Thriller .
Not all the episodes are worth watching but there are some very good ones like : Pigeons From Hell, A Wig For Miss DeVore, The Hungry Glass, The Cheaters, The Grim Reaper .
Plus you get to see people who later became quite famous like William Shatner, Russell Johnson, Dick York, Mary Tyler Moore.