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To overcome the biological barriers formed by the lignin–carbohydrate complex for releasing fermentable sugars from cellulose by enzymolysis is both imperative and challenging. In this study, a strategy of intergranular swelling of cellulose combined with hydrolysis and oxidation was demonstrated. Pretreatment of the bagasse was evaluated by one bath treatment with phosphoric acid and hydrogen peroxide. The chemical composition, specific surface area (SSA), and pore size of bagasse before and after pretreatment were investigated, while the experiments on the adsorption equilibrium of cellulose to cellulase and reagent reuse were also performed. Scanning electron microscopy (SEM) and high-performance liquid chromatography (HPLC) were employed for microscopic morphology observations and glucose analysis, respectively. The results showed that pretreated bagasse was deconstructed into cellulose with a nanofibril network, most of the hemicellulose (~100%) and lignin (~98%) were removed, and the SSA and void were enlarged 11- and 5-fold, respectively. This simple, mild preprocessing method enhanced cellulose accessibility and reduced the biological barrier of the noncellulose component to improve the subsequent enzymolysis with a high glucose recovery (98.60%).