Had to ponder on this for a while, difficult choice as I like them all! In the end I plumped for From Beyond the Grave. For sheer creepiness I would have to select "Act of Kindness" as the best story, with Ian Bannen and a terrific turn from Donald and Angela Pleasence.
My DIY Amicus would consist of:
"Act of Kindness" - Ian Bannen, Donald and Angela Pleasence.
"The Cloak" - Jon Pertwee and Ingrid Pitt.
"The Door" - Ian Ogilvy, Jack Watson and Lesley Anne-Down
"Blind Alley's" - Nigel Patrick, Patrick Magee.
"Poetic Justice" - Peter Cushing.

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Could be, he certainly had bushmungus eyebrows enough to put the willies up the lot of them. 