Sugarcane bagasse and rice straw are major agricultural byproducts often discarded or burned as waste after cultivation, leaving their untapped potential for utilization. In this work, cellulose fibers were extracted from sugarcane bagasse and rice straw using a simple procedure: alkaline treatment with sodium hydroxide, bleaching with sodium hypochlorite, and acid hydrolysis. The obtained cellulosic materials were successfully prepared into milky white and transparent films, of which the transparency slightly decreased with the addition of glycerol. The surface of all the films appeared homogeneous with a random orientation of fibers. The rice-straw (RS) film had a more fragile texture than the sugarcane-bagasse (SBG) film. The FTIR analysis clearly indicated the functional groups of cellulose, as well as glycerol for the films mixed with glycerol. Thermal analysis showed that the native SBG film decomposed at 346 °C, higher than the native RS film (339 °C). The presence of glycerol in the films resulted in slightly lower maximum decomposition temperature (Td,max) values as well as mechanical properties. Regarding water susceptibility, the RS film had a higher percentage than the native SBG and glycerol-mixed SBG films. The extracted cellulose from both sources could form almost spherical-shaped cellulose particles. Thus, through the simple extraction method, sugarcane bagasse and rice straw could serve as excellent sources of cellulose materials for preparing cellulose films and particles, which would be advantageous to the development of cellulose-based materials.