Whereas cellulose-derived polymers are routinely used as membrane materials, the cellulose polymer itself is not directly used to synthesize dense/porous films for membrane applications. Recently, N-methylmorpholine N-oxide (NMMO) and din-iethylacetamide (DMAc)/Iithium chloride (LiCl) have been successfully employed for dissolving unmodified cellulose. This provides a strong rationale for reexamining the possibility of cellulose membrane fabrication using these solvents. By judiciously selecting solvents, casting conditions, and solvent exchange steps, we successfully synthesized dense/asymmetric-porous cellulose films. The pore size and porosity of the porous films decreased systematically with increasing cellulose concentration. SEM analysis of the cross sections revealed an asymmetric skinned structure with monotonically increasing pore size away from the skin. The measured pore diameters were in the range 1.8-4.8 pm. Mechanical testing indicated that the dense films possessed tensile properties comparable to those of cellulose acetate (CA) films. Though nitrogen permeability values were comparable for cellulose and CA dense films, cellulose film permeability depended upon the type of drying protocol employed. Overall, these results demonstrate that processability need not be a constraint in the use of cellulose polymer for membrane fabrication. In selected applications, cellulose membranes could become a cost-effective, environmentally friendly alternative to other more commonly employed membrane polymers. (c) 2007 Wiley Periodicals, Inc.