We systematically investigate the assembly of multilayers based on a polyzwitterion (PSBMA) and a polycation (PDADMAC) for the development of ionic strength responsive membranes. Although the polyzwitterion is essentially charge neutral, we show that specific electrostatic interactions with the PDADMAC allow for the formation of stable multilayers. The growth of this LbL system is monitored on model surfaces (silica) via optical reflectometry for different pH values and ionic strengths. While no effect of pH on the layer growth is observed, we did observe a strong dependence on the ionic strength. Upon increasing the ionic strength during deposition from 0.005 to 0.5 M NaCl, the adsorbed amount is significantly decreased, a behavior that is opposite to classical LbL systems. Similar results to those obtained on silica are also observed on top of classical LbL systems and on polymeric membranes. This demonstrates that the growth of the polyzwitterion multilayers is independent of the substrate. Coating these polyzwitterion multilayers on hollow fiber membranes via dip-coating yields membranes that are stimuli responsive toward the ionic strength of the filtration solution, with an increase in permeability of up to 108% from 0 to 1.5 M NaCl. We show that the fabrication of the polyzwitterion multilayers is an easy and controlled way to provide surfaces, such as membranes, with the specific functionalities of polyzwitterions.