Beyond conventional porous materials, metal–organic frameworks (MOFs) have aroused great interest in the construction of nanocatalysts with the characteristics of catalytically active nanoparticles (NPs) confined into the cavities/channels of MOFs or surrounded by MOFs. The advantages of adopting MOFs as the encapsulating matrix are multifold: uniform and long‐range ordered cavities can effectively promote the mass transfer and diffusion of substrates and products, while the diverse metal nodes and tunable organic linkers may enable outstanding synergy functions with the encapsulated active NPs. Herein, some key issues related to MOFs for catalysis are discussed. Then, state‐of‐the art progress in the encapsulation of catalytically active NPs by MOFs as well as their synergy functions for enhanced catalytic performance in the fields of thermo‐, photo‐, and electrocatalysis are summarized. Notably, encapsulation‐structured nanocatalysts exhibit distinct advantages over conventional supported catalysts, especially in terms of the catalytic selectivity and stability. Finally, challenges and future developments in MOF‐based encapsulation‐structured nanocatalysts are proposed. The aim is to deliver better insight into the design of well‐defined nanocatalysts with atomically accurate structures and high performance in challenging reactions.