Supported metal nanoparticles (NPs) catalysed chemical transformations have been a vital area of research over the last few decades. Catalysis by supported NPs not only plays a pivotal role in the production of fine chemicals such as coupling products, heterocycles, alcohols, carbonyl compounds, acids, etc. but also provides sustainable chemical processes. The use of supported metal NPs provides a much prosperous basis than conventional homogeneous and heterogeneous catalysts for tuning reactivity, recyclability, high productivity and environment benevolent alternative for C−H functionalization. Consequently, as evidenced in the literature, various support materials such as silica, metal oxides, zeolites, carbon‐based materials, bio‐materials, magnetic materials, and MOFs have been moderately investigated in order to exploit their benefit in supported metal NPs catalyzed various C−H functionalizations. This review aims to summarize recent advances in the development of new support materials or novel supported NPs catalytic systems for functionalization of the challenging C−H bond under heterogeneous conditions. Furthermore, a deep scientific understanding of the mechanisms, active species, role of base and oxidants for these systems are also discussed to gain insight into the advance in the rational design of efficient catalytic systems, which may serve as an inspiration to researchers in their future work.