To answer the actual TOD is challenging, but looking at Wikipedia's list, here goes:
Cape Fear
Carnival of Souls
David and Lisa
Dr. No
Experiment in Terror
Gypsy
How the West Was Won
Lawrence of Arabia
Lolita
The Longest Day
The Manchurian Candidate
The Miracle Worker
Mr. Hobbs Takes a Vacation
The Music Man
Mutiny on the Bounty
Requiem for a Heavyweight
To Kill a Mockingbird
What Ever Happened to Baby Jane?
There are others I like or love equally as well, but those are the clear leaders. Those others would be several from Roger Corman (including The Intruder which I only became acquainted with a couple of years ago), Birdman of Alcatraz, Confessions of an Opium Eater, Days of Wine and Roses, The Man Who Shot Liberty Valance, Panic in Year Zero!, Ride the High Country, and Two for the Seesaw. These are all movies I can watch repeatedly, like the above.