In this work, the hydrogen storage behaviors of carbon nanotubes (CNTs)/metal-organic frameworks-5 (MOF-5) hybrid composites (CNTs/MOF-5) were studied. Hydrothermal synthesis of MOF-5 was conducted by conventional convection heating using 1-methyl-2-pyrrolidone (NMP) as a solvent. Morphological characteristics and average size of the CNTs/MOF-5 were also obtained using a scanning electron microscopy (SEM). The pore structure and specific surface area of the CNTs/MOF-5 were analyzed by N2/77 K adsorption isotherms. The capacity of hydrogen storage of the CNTs/MOF-5 was investigated at 298 K/100 bar. As a result, the CNTs/MOF-5 had crystalline structures which were formed by hybrid synthesis process. It was noted that the CNTs/MOF-5 can be potentially encouraging materials for hydrogen adsorption and storage applications at room temperature.