The advances made in the mechanosynthesis of inorganic and organometallic complexes and the excellent past developments with metal-catalyzed cross-coupling reactions by high-speed ball milling have sufficienly laid the ground work for the merging of C-H functionalization and mechanochemical techniques. In recent years, the fast development of mechanochemical C-H activation have given us examples of metal-catalyzed olefinations, amidations, halogenations, and oxidative couplings, among others. This concept article will describe some of the events that led to the development of mechanochemical C-H activation, the current state-of-the-art, the present challenges of this merge, and some unique scenarios in which mechanochemistry could complement the traditional solution-based approaches.