Melamine formaldehyde (MF)-functionalized cellulose nanocrystals (CNC) prepared via an in situ polycondensation reaction were incorporated into hardwood pulp (HWP) membrane filters to remove anionic contaminants in water. Batch adsorption experimental data were fitted to the Freundlich model, yielding a capacity of 80 mg/g for methyl orange (MO), and the adsorption capacity was enhanced at higher temperatures. The incorporation of MF-CNCs in HWP membranes up to 14 wt % resulted in a 6-fold improvement in the wet strength and greater dye removal. However, the inclusion of MF-CNCs reduced the flux through the membranes due to the reduction of the pore size. Using a custom-designed filter cartridge, up to 20 layers of MF-CNC incorporated HWP membranes were stacked and operated at a flow pressure of up to 30 psi. Filtration studies confirmed that MF-CNCs readily bind MO inside the HUN matrix, making them effective filtration media. Functionalized CNC-incorporated HWP membranes hold great promise for the removal of a wide variety of contaminants. The simplicity and low cost in preparing and using these membranes for the removal of contaminants make this system suitable for a point-of-use water treatment system.