No one could act irritated in a "superior" way better than Ray Milland, so Jarvis Goodland is a great one.
She’s not a murderer (despite threats to kill Columbo) but the all time Most Irritated By Columbo Award goes to.......Mrs. Peck. .
At one point in THE MOST CRUCIAL GAME, Robert Culp is so annoyed he sounds genuinely whiny instead of angry. It's that line "Columbo, what IS IT?!"
"Columbo I'm gonna THROW YOU OUTTA HERE! ON YOUR EAR!"