I haven't watched it but I've heard that Chaos;Head is a very bad adaptation which is evident even to non VN players (in contrast to Steins;Gate) but I am watching Guilty Crown and I can say that it's only worth watching for it's impressive production values and little else. It is exciting if you turn your brain off a bit but it hasn't finished airing so it'll be a while if you still want to watch Chaos;Head. I'd go with Chaos;Head first.
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