AbstractMoso bamboo (Phyllostachys edulis) is an important source of lignocellulosic materials because of its fast growth, its vegetative propagation, and its easy harvesting. The pretreatment of bamboo with dilute sulfuric acid and the effects on its chemical components and enzymatic hydrolysis were studied, in addition to the fibrous structural properties of pretreated residues by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared (FTIR) spectroscopy. The results showed that dilute sulfuric acid pretreatment primarily hydrolyzed hemicelluloses and resulted in enhanced cellulose and lignin content in the pretreated solids. The maximum yield of hemicellulose recovery was 81.42% when pretreated with 1.00% sulfuric acid at 150 °C for 30 min, and the enzymatic hydrolysis yield was 79.45% when hydrolyzed for 72 h with an enzyme loading of cellulase 40 FPU/g of cellulose. Under these conditions, the overall sugar yield was 83.36% (cellulose and hemicellulose), with a total of 67.11 g fermentable sugars from 100 g dry bamboo. The results indicated that Moso bamboo underwent considerable changes in its chemical composition and physical properties after acid pretreatment, such as the removal of hemicellulose and lignin, an increase in specific surface area and pore volume, and exposure of internal structure, which enhances the enzymatic hydrolysis of Moso bamboo.