Activated carbons (ACs) were developed from the agricultural by-products of moso bamboo by pyrolysis carbonization and the KOH activation process. N2 adsorption-desorption at 77 K, thermogravimetric analysis (TG), X-ray photoelectron spectrometry (XPS), element analysis (EA), X-ray diffraction (XRD), scanning electron microscopy (SEM), high- resolution transmission electron microscopy (HRTEM), and Fourier transform infrared spectroscopy (FTIR) were used to investigate the synthesis process, the impact of the weight ratio of KOH/bamboo charcoal (BC), and the characteristics of the bamboo charcoal and ACs produced. The results showed that the developed bamboo ACs achieved surface areas (SBET) as high as 3208 m2/g and micropores volumes (VDR) as high as 1.01 cm3/g. The carbonation and activation of the bamboo resulted in the enhancement of the microstructure of the bamboo ACs, and hence improvements in the sorption behavior and storage capacity. The highest hydrogen storage capacities achieved were 6.6 wt.% at 4 MPa and 2.74 wt.% at 1 bar, both at 77 K, which were much higher than those of a well-known commercial activated carbon.