Advances in capacitors, batteries, actuators, ion-transport membranes, sensors and triboelectric nanogenerators require materials with high dielectric constants (ε_s). Synthesis of high ε_s soft materials is currently approached by three methods: 1) swelling polymeric materials with high dielectric constant polar liquids, 2) addition of inorganic fillers, or 3) chemically modifying materials with polar substituents. Although there has been success with increasing ε_s in materials, the increases in ε_s have been minimal, the additives/functional groups negatively affect the mechanical properties, and/or there is a reduction in the breakdown strength. An alternative approach is to add zwitterionic liquids (i.e., dielectricizers) that exhibit exceptionally high dielectric constants with negligible volatility. The presentation will discuss the connection between zwitterionic molecular modifications and dielectric constant, demonstrating that it is possible to achieve one of the highest dielectric constants among all liquids (~ 350 at 293 K). The main molecular tuning parameters for maximizing zwitterionic liquid dielectric constant are increasing the cation-anion linkage length and using delocalized charged groups, leading to an enlargement of the molecular dipole and a homogenous liquid morphology, respectively. Zwitterion modifications to polymers also increases the dielectric constant of soft materials. Covalently attaching high ε_s zwitterions into polymer networks will help with processing while maintaining desired mechanical properties. Functionalizing polymers with zwitterionic side groups increases ε_s by 2X (e.g., 5 → 10), which is significant, but less than the upper limit predicted knowing the zwitterion mole fraction in the polymer. Expanding the scope of high ε_s materials to zwitterionic polymers will enable tuning of performance using zwitterion chemistry as well as polymeric material composition and thermomechanical properties. The extremely high dielectric constant accessible with zwitterions paves new avenues for dielectric polymer materials.