Sterling Hayden
Down and out. What’s a smile.
Leo Gordon
Leo never learned how to. Well you can’t when you’re the permanent baddie.
Dana Andrews. THE BEST YEARS OF OUR LIVES
He will smile again.
Ella Raines. PHANTOM LADY
She will too. But she is on a mission just now.
Charles Middleton. MING THE MERCILESS
He cant smile. Think of the image.
Bogie can, when he wants to.
John Payne.99 RIVER STREET
What could I possibly smile about. I’m on the run from the police. They think I killed my wife.
Lionel Barrymore.IT’S A WONDERFUL LIFE
I do grumpy, not grins.
Robert Ryan
It’s really, really hard for Robert.
Edward G Robinson
Oh, gimme a break. I ain’t smiling for nobody.
Robert Mitchum.Night of the Hunter
You want me to what?
Vienna's Classic Hollywood 
Sterling Hayden has the saddest mouth. Edward G. can pull quite a grimace himself, though.
You’re right. I’ve added Edward G. to the lineup.