In this work, nickel (Ni)-loaded activated carbon nanotubes (ACNTs) were prepared for hydrogen storage applications. The process was conducted by chemical activation method at 900oC with KOH:CNTs ratios (4:1, g/g). And then, Ni-loaded ACNTs were also formulated to investigate the hydrogen storage characteristics as a function of Ni content. The microstructures of the Ni-loaded ACNTs were characterized by XRD and TEM measurements. The textural properties of the samples were analyzed using N2 adsorption isotherms at 77 K. The BET, D-R, and BJH equations were used to observe the specific surface areas, the micropore, and mesopore structures, respectively. The hydrogen storage capacity of the Ni-loaded ACNTs was measured at 298 K at a pressure of 100 bar. It was found that the hydrogen storage capacity of Ni-loaded ACNTs was enhanced in proportion to the Ni content, with Ni-5-ACNTs exhibiting the largest hydrogen storage capacity. Therefore, it could be concluded that the significantly created micropores on CNTs by chemical activation had an effect on hydrogen storage behaviors as well as the Ni particles played an important role in hydrogen storage characteristics due to the hydrogen spillover effect.