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Grayson the Armourer is the one with the most chances of dropping books. Most of them have a high chance for an unsullied heart. But all in all, I don't see many reasons to farm bosses, going towards a press to unlock all recipes via paper is less of a hassle.
You're right. Crates and other objects have a chance to drop materials (sometimes, even rare ones like gold jewels and recipe books, so it's always a wise strategy to break everything you come across.
they use to drop them fairly regularly, now it's quite rare as the primary source for them was changed to rift incursions and stygian vendors.