Cellulose-ZnO nanolayer film (CZNF) was prepared by simply mixing ZnO nanopowder with cellulose solution and sodium dodecyl sulphate dispersing agent. CZNF was cured in a mixture of isopropyl alcohol and deionized water and a freestanding film was obtained. CZNF was prepared with different weight percentage of ZnO and all materials were characterized by optical, thermal, mechanical and electrical methods. The morphology shows that ZnO nanoparticles are evenly dispersed between cellulose nanolayers of CZNF. Thermal and mechanical test results exhibit that CZNF possesses two distinctive characteristics of regenerated cellulose and ZnO. Its complex electrical impedance exhibits very similar to ionic membranes for fuel cells.