Antiferroelectric materials exhibit a unique electric-field-induced phase transition, which enables their use in energy storage, electrocaloric cooling, and non-volatile memory applications. However, in many prototype antiferroelectrics this transition is irreversible, which prevents their implementation. In this work, we demonstrate a general approach to promote the reversibility of this phase transition by targeted modification of the material's local structure. A new NaNbO3-based composition, namely (1-x)NaNbO3-xSrSnO3, was designed with a combination of first-principles calculations and experimental characterization. Our theoretical study predicts stabilization of the antiferroelectric state over the ferroelectric state with an energy difference of 1.4 meV/f.u. when 6.25 mol.% of SrSnO3 is incorporated into NaNbO3. A series of samples was prepared using solid state reactions and the structural changes upon SrSnO3 incorporation were investigated using X-ray diffraction and 23 Na solid-state nuclear magnetic resonance spectroscopy. The results revealed an increase in the unit cell volume and a more disordered, yet less distorted local Na environment, which were related to the stabilization of the antiferroelectric order. The SrSnO3-modified compositions exhibited well defined double polarization loops and an 8times higher energy storage density as compared to unmodified NaNbO3. Our results indicate that this first-principles calculations based approach is of great potential for the design of new antiferroelectric compositions.