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The Darkhold first appeared in Marvel Comics in 1972 in the 4th issue of the 1st volume of Marvel Spotlight.
Background
The Darkhold is an evil book which consists of the scrolls of Chthon. Hundreds of millions of years ago, when he and nearly all of his fellow Elder Gods became corrupt, murdering each other and practicing dark forbidden arts, he wrote down all of his dark knowledge in indestructible parchment. Which was due to their coming defeat and annihilation at the hands of the Demigorge, a god-eating god given birth by the goddess Gaea to cleanse Earth of their evil. He fled into a parallel dimension that he created, leaving it behind on Earth to provide him a link back to his homeworld.
Within the Darkhold is great power. Chaos magic which can create random chaotic (destructive, and lethal) effects across the Earth, and when used by Chthon himself, it can reshape the world itself. Necromantic magic that whenever used in the history of mankind has destroyed civilizations. Spells that have created vampires, zombies, and werewolves. Various dark cults and sorcerers have used the book down the ages, including Atlantean sorcerers who became the world's first vampires. The infamous Necronomicon is actually based on the Darkhold, and only contains within it a small fraction of the dark knowledge of the Darkhold.