Faced with a pressing need for membranes with a higher permeability and selectivity, the field of membranetechnology can benefit from a systematic framework for designing membranes with the necessaryphysical characteristics. In this work, we present an approach through which transport modeling is employedin fabricating specialized nanofiltration membranes, that experimentally demonstrate enhanced selectivity.Specifically, the Donnan-Steric Pore Model with dielectric exclusion (DSPM-DE) is used to probefor membrane properties desirable in desalination pretreatment. Nanofiltration membranes are systematicallyfabricated in-house using layer-by-layer (LbL) deposition to validate model predictions and to develop anew specialized membrane for this application. The new membrane presents a 30% increase in permeabilityand a 50% reduction in permeate hardness relative to state-of-the-art NF membranes. Our results indicatethat a ‘specialized’ tight membrane can outperform looser counterparts in both permeability and selectivity.Given the possibility of extending this framework to other applications, the work furthers our understandingof the relationships governing membrane form and function, while having broad potential implications forfuture nanofiltration membranes used in chemical separation and purification.