Having used both, I have to cast my vote for Chaosium. D20 is simpler, but in this case, simpler is relative and not necessarily the best way to play HPL's mythos. And, if you haven't tried playing the original D&D in a while, then take a look at it and
then tell me it's "less complicated" than Chaosium's CoC!
As someone else points out, using D20 would allow you to turn a CoC campaign into a "Monty Haul" version of HPL's vision, but using Chaosium's CoC forces the players to really think and roleplay, since not only are guns deadly, but sanity loss is a real risk.
Plus the sheer quality of Chaosium's design work and scenario packs is a thing of beauty. All things considered, I prefer "classic" CoC versus the D20 design.
I did take a look at "Realms of Cthulhu" but after spending over $20 for it, I found only ONE good idea in the whole thing -- the rest just adapts the CoC system, which doesn't really lend itself that well to adaptation.
Finally, there is "Trail of Cthulhu" which adapts CoC to the "Gumshoe" system. Really the only innovative part there is that in "Gumshoe" you always find the clue you need! While that's good for some clues, it's also nice to have the players proceed with a few gaps in their knowledge -- especially if you can make them suspicious there might actually BE such a gap -- it tends to increase paranoia and fear -- both of which are sort of crucial to a good CoC campaign!
