I voted for Miss Cathcart, Sgt. Mooney, Mr. Krinkie and Grandma Mitchell in that order.
Without looking, George Cisar as Mooney was in considerably more episodes than any of the other three but like Mary Wickes, both stole every one of their scenes.
I was never a fan of Mrs. Elkins. Outside her earliest appearances, she was nasty with no real reason to be. I never blamed either Wilson brother for disliking her.
And it's funny about Mr. Dorfman, Mrs. Holland, Opie and even Joey that they made semi-regular appearances in the first season and were never seen again but still mentioned after they last were seen. In Joey's case, he was mentioned all the way in the third-to-last episode even though we hadn't seen him in almost four years.
[ETA: Per IMDB, Mooney was in 31 episodes, Elkins 26, Cathcart 10, Krinkie 9 and Grandma Mitchell 8.]
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