As two coexisting and fast-growing research fields in modern synthetic chemistry, the merging of organocatalysis and C-H bond functionalization is well foreseeable, and the joint force along this line has been demonstrated to be a powerful approach in making inert C-H bond functionafization more viable, predictable, and selective. In this review, we provide a comprehensive summary of organocatalysis in inert C-H bond functionalization over the past two decades. The review is arranged by types of inert C-H bonds including alkane C-H, arene C-H, and vinyl C-H as well as those activated benzylic allylic C-H, and C-H bonds alpha to the heteroatom such as nitrogen and oxygen. In each section, the discussion is classified by the explicit organocatalytic mode involved.