There has been an increasing interest in recent years in isolating cellulose nanofibers from unbleached cellulose pulps for economic, environmental, and functional reasons. In the current work, cellulose nanofibers isolated from high-lignin unbleached neutral sulfite pulp were compared to those isolated from bleached rice straw pulp in making thin-film ultrafiltration membranes by vacuum filtration on hardened filter paper. The prepared membranes were characterized in terms of their microscopic structure, hydrophilicity, pure water flux, protein fouling, and ability to remove lime nanoparticles and purify papermaking wastewater effluent. Using cellulose nanofibers isolated from unbleached pulp facilitated the formation of a thin-film membrane (with a shorter filtration time for thin-film formation) and resulted in higher water flux than that obtained using nanofibers isolated from bleached fibers, without sacrificing its ability to remove the different pollutants. Membranes are used in a wide variety of industries for removing undesirable materials from different media. Among them, those that depend on separation based on the size of materials to be removed, e.g., micro-, ultra-and nano-filtration membranes, are manufactured using different polymers; generating pores within these membranes with targeted size is the key for their use 1. Using cellulose and its derivatives for making membranes for use in micro-and ultrafiltration is well known at the commercial level 2. Cellulosic membranes are usually prepared using casting technique, which depends on the dissolution of cellulosic materials in suitable solvents, followed by film formation by immersion in a non-solvent. This technique requires use of large amounts of solvents; their recovery is important for economic and environmental reasons. Since the emergence of nanocellulosic materials, e.g., cellulose nanofibers and cellulose nanocrystals, increasing research is ongoing regarding their use in the area of membranes. Two approaches have been investigated for use of nanocellulose in that area so far 3. The first approach is through their incorporation in other polymer matrices to improve the performance of prepared membranes. Dissolving the polymers in suitable solvents and also good dispersion of nanocellulosic materials in the polymer solution are necessary before film casting. The second approach studied, which is more favorable and interesting, is to make membranes from a layer of nanocellulose with adequate porosity over other polymeric supports without the need to dissolve the cellulose and to use the film casting technique to generate porosity. The second approach was first introduced by Ma et al. 4 ; it depends on the correlations between pore size distribution of a nonwoven layer structure and bulk porosity. According to this approach, the pore size of a film made from fibers can be adjusted by controlling the fiber diameter. It was also proved through a study of the pore size of films made from electrospun nanofibers that the mean pore size was found t...