Nanofiltration (NF) membranes typically carry a net electric charge, enabling electrostatic interactions to play a pivotal role in the rejection of species such as metals, nitrates, and other charged contaminants. In this study, two types of polymeric NF membranes, polyamide and cellulose acetate, were modified by ion implantation to increase the effective surface charge of the membranes. The modified membranes contain implanted ions in the membrane matrix, inducing a discrete, permanent charge in the active membrane layer. The presence of a permanent charge in the membrane matrix allows for increased electrostatic repulsive forces throughout the entire pH range. Streaming potential measurements were conducted as a function of pH for the modified and unmodified membranes to determine the effect of ion implantation on the zeta potential of the membranes. Rejection experiments were performed in order to quantify the effect of increased electrostatic repulsion on ion rejection, and flux measurements quantified the effect of the modification on permeability. Results indicate that electrostatic interactions near the membrane surface can affect rejection; however, the extent of the effect of increased membrane charge depends on physical-chemical characteristics of the membrane. Increased negative zeta potential of the modified membranes resulted in slightly higher rejection of salts with divalent co-ions from the membrane, with less increase observed with salts of monovalent co-ions. Modified membranes were less permeable than the unmodified membranes. Results of this research hold implications in membrane synthesis and modification studies as well as choice of membranes for water treatment applications.