There is no bone in the human brain. The brain is a soft organ protected by the skull, which is made up of multiple bones. If the question meant to ask "Which is the largest bone of the skull?", the answer is the mandible (jawbone).
The skull comprises two main parts:
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Cranium (Neurocranium): This bony structure protects the brain.
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Mandible (Viscerocranium/Facial Skeleton): This is the lower jawbone, and it is the largest and strongest bone in the face.
Therefore, while not in the brain, the largest bone associated with the skull and protecting the brain is the mandible.