Solid chemisorption technologies for hydrogen storage, especially high-efficiency hydrogen storage of fuel cells in near ambient temperature zone defined from −20 to 100°C, have a great application potential for realizing the global goal of carbon dioxide emission reduction and vision of carbon neutrality. However, there are several challenges to be solved at near ambient temperature, i.e., unclear hydrogen storage mechanism, low sorption capacity, poor sorption kinetics, and complicated synthetic procedures. In this review, the characteristics and modification methods of chemisorption hydrogen storage materials at near ambient temperature are discussed. The interaction between hydrogen and materials is analyzed, including the microscopic, thermodynamic, and mechanical properties. Based on the classification of hydrogen storage metals, the operation temperature zone and temperature shifting methods are discussed. A series of modification and reprocessing methods are summarized, including preparation, synthesis, simulation, and experimental analysis. Finally, perspectives on advanced solid chemisorption materials promising for efficient and scalable hydrogen storage systems are provided.