Loved those episodes with him as Mudd, and especially that one. The personification of a "lovable fraud".
When my brother's wife started to nag him (often) he would raise his arm, point at her and just say "Harcourt" in that grating voice. It got to be an inside family joke in that any time we ran across a harpy, we'd just look at one another and in a high-pitched voice, say "Harcourt!".
I still prefer the original series above all the others, where every alien was usually just a humanoid in makeup.
The actress who really turned me on was Yvonne Craig in "Whom the Gods Destroy" - she looked like she would hurt me - and I wouldn't care - cold showers all week: 
and
Marta