This work investigates the evolution of cellulose crystals from sugarcane lignocellulose (bagasse and leaves) submitted to prehydrolysis (hydrothermal, dilute acid, or steam explosion) and soda delignifications. Raw and treated materials are characterized by X-ray diffraction with modeling of area-detector patterns. Three treatment effects are correlated: increase in cellulose content, quantified by strong acid hydrolysis; increase in average cellulose crystallite width, inferred from sharper 200 diffraction peaks; and decrease in crystallite distortion, evidenced by d 200-spacing approaching reference values. Crystal contents measured according to recent developments (in Driemeier and Calligaris, J Appl Cryst 44:184–192, 2011) are compared to cellulose contents. Limitations for this comparison are discussed. Results are consistent with minimum non-crystalline cellulose in raw lignocellulose, and with partial cellulose decrystallization or more defective crystallites in treated materials.