
Perpdepog |
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While it's a resource for PF1E, you can probably get a lot of mileage out of Horror Adventures. It has lots of system-agnostic advice for ways to run horror-themed campaigns, and has a sanity system as well. I don't know how well that'll translate over to 2E given the differences in numbers, but I think it should still be a good starting point.
As for Cthulhu specifically, he is a deity in the setting, and has a little written about his domains and church, though it's sadly 1E information again.
If you have skill, or know someone with skill, at converting over monsters to 2E from 1E then I'd also recommend checking out the various monsters from the Strange Aeons adventure path, which was the Lovecraftian, eldritch-themed AP.

Claxon |
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One thing to make sure of is that your players are on board with these kinds of systems/game.
One I love Pathfinder, the inexorable dread of going mad in Call of Cthulhu is something I hate. If you told me in advance you were planning to run that kind of game, I would decline to play.
If you were to spring it on me after play had started I would be resentful, stick it out for a while (making everyone's play experience worse), until I finally reached a breaking point and quit.

keftiu |
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Pathfinder 2e is a game about magical heroes who solve their problems with violence. You're going to be fighting against the current some to make an Elf Wizard or an Automaton Barbarian feel as fragile as a 1920s Investigator, so be well aware that "see the Mythos and go beat up on it" is going to be the most functional flavor you land on. It's not impossible - 1e's Strange Aeons and 2e's Malevolence prove you can do cosmic horror here - but there's definitely easier ways.
Can I ask why you want to hack Pathfinder, rather than using one of dozens of existing Cthulhu rulesets?

Castilliano |
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As implied by the others, that "dread" portion's the toughest in any RPG as you have to balance around player investment in their PCs, as in many are reluctant to develop a disposable PC or run their developed PCs through the ringer every session. Which as mentioned above means you need to check that your player base enjoys horror (despite how cool it might seem to surprise them). There's an amount of emotional buy-in required that many don't want to pay during their fun time.
(Read Lovecraft's On the Nature of the Supernatural (free online) to help both with understanding this and putting yourself in this kind of creative mindset!)
You don't want the obstacles/fear to be brute force, merely about the numbers or disadvantages so yeah, look into horror-themed RPG advice in Cthulhu or Ravenloft products, where atmosphere and storytelling matter much more. Same goes for Planescape (2.0) to a degree as well as Deadlands, both of which have insurmountable enemies one must operate around and thwart yet can never directly confront (or even hope to confront). And Deadlands also has a fear system with repercussions.
And as keftiu mentioned, heroic fantasy's main conceit (heroic PCs make major impacts through direct confrontations) conflicts with the horror genre (hapless characters struggle for survival). Heck, one rule of thumb in the horror RPGs is that the "treasure reward" is living intact and sane (which conflicts with the treasure-based power increases in PF & many games).
So you have to figure out how much you want to lean into this. The Strange Aeons AP is likely the best middle-ground to begin if you're thinking in Pathfinder terms (and would be simpler to adapt into 2.0 than starting from scratch), while if coming from the horror side then yeah, you might want to begin with another system (even if you return to PF after consideration).
As for me, I ran a Deadlands game which adapted heavily from Ravenloft and used many Hero System scenarios. All three meshed remarkably well because mechanics were tertiary to plot and atmosphere.