Objective： This study focus on preparing microcrystalline cellulose with high adsorption capacityfromcoffee shells. Methods: Acid hydrolysis method was employed to prepare microcrystalline cellulose and the effects of acid hydrolysis time, acid hydrolysis temperature, percentage of acid and the ratio of material to solvent on the yield and adsorption capacity of microcrystalline cellulose were investigated. Furthermore, orthogonal experiment was taken to optimize the process parameters. Results: The optimum preparation conditions of coffee shell microcrystalline cellulose were as follows: acid hydrolysis time of 95 min, hydrochloric acid mass fraction of 16%, material to solvent ratio of 1∶22 （g/mL） and acid hydrolysis temperature of 60 ℃. Under the control of these conditions, the yield of coffee shell microcrystalline cellulose was 80.08%, and the flavor adsorption capacity of which was 0.89 g/g. Conclusion: The material to solvent ratio had the greatest influence on the yield of coffee shell microcrystalline cellulose, and the acidolys temperature had the greatest influence on its adsorption capacity. Coffee shell microcrystalline cellulose with highest yield and adsorption was obtained under the optimized process.