New materials with potential applications for adhesives and coatings, based on copolymers containing zwitterionic pendent groups, were investigated. n-Butyl acrylate and 2-ethoxyethyl acrylate were copolymerized with a series of five zwitterionic sulfobetaine monomers (SBMs). The structures of the SBMs were varied systematically in terms of (1) intercharge spacing in the zwitterionic moiety and (2) substituent bulkiness at the quaternary ammonium functionality. The effect of varying the sulfobetaine content and structure in the copolymers was investigated, with an emphasis on ion aggregation behavior and physical properties, with dynamic mechanical analysis. The zwitterionomers exhibited the expected biphasic morphology, with the appearance of an ion-rich glass-transition temperature. An increase in the storage modulus was observed with increasing SBM content in the rubbery and terminal regions, suggesting an increased degree of ionic crosslinking in the rubbery region and decreased chain mobility in the flow region. Intercharge spacing variation in the sulfobetaine moiety did not have a significant effect on the modulus-temperature curves, contrary to our expectations. Increases in the modulus were much less pronounced for the bulkier SBMs than for the other monomers, possibly because of hindered aggregation of the sulfobetaine moieties. Likewise, matrix polarity had a greater influence on the physical properties of these materials than intercharge separation in the SBMs.