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What a great question.
T.B.H. a tricky question too as there have been so many episodes!
If we just concentrate on scooby-doo where are you the original with 29 villians in that series. I would have to say the Black knight from the original episode set the mood and bar for future villens to come.
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The other would be The Mummy of Ankha
If I'm honest I was more captivated as a kid by the chase scenes and my velma then the criminal, spooky villian; who you came to expect their cumuppance by the end of the episode.
Thanks for the question.
Made me think and have to check my old vhs collection lol.
R.I.P. Joe Ruby. Co created of scooby-doo. Who passed away today aged 87.