Zincoxen cellulose solution was used as raw materials for the preparation of zincoxen/cellulose complex microspheres via a spray drying process. The obtained zincoxen/cellulose microspheres were turned into assemblies of ZnO nanocrystals upon calcinations at 500 or 700 . The assemblies of ZnO nanocrystals exhibit high photocatalytic activity for methyl orange degradation under ultraviolet light irradiation in aqueous solution and also satisfied reusability and stability of morphology and composition.Page 3 of 24 A c c e p t e d M a n u s c r i p t Highlight Spray drying technique was utilized for the preparation of ZnO nanocrystal assemblies using zincoxen cellulose solution as raw materials.Zincoxen plays both the role as solvent for cellulose and precursor for the ZnO nanocrystals.Cellulose acts as assembly agent during the spray drying step and sacrificial templates in the calcinations processThe content of cellulose and the calcination temperature influence the properties of the resulted ZnO nanocrystal assembliesThe assemblies of ZnO nanocrystals exhibit high photocatalytic activity for methyl orange degradation in aqueous solution.Page 4 of 24