Abstract: The present disclosure provides a surface-nanocrystallized cellulose-containing biomass material, a preparation method and use thereof. The cellulose-containing biomass material is one or more derived from biomass materials containing cellulose components from natural plants or animals. Nanoscale celluloses are present on a surface of the surface-nanocrystallized cellulose-containing biomass material, and a portion of hydroxyl groups in the cellulose structure has been converted to carboxyl groups, such that the surface-nanocrystallized cellulose-containing biomass material has high specific surface area, high surface activity, and high crystallinity. Thus, the present application provides an excellent raw material for the further processing of biomass materials.