Lead-free antiferroelectric ceramics have drawn widespread interest recently on account of their environmentally friendly components and potential applications in high-power systems. However, their relatively low recoverable energy storage density (W rec < 10 J/cm 3 ), limited by the electric breakdown strength (E b < 60 kV/mm), and low efficiency (η < 80%), generated by large hysteresis during the antiferroelectric−ferroelectric phase transition, have seriously restricted their application in portable and compact electronic devices. In this study, the relaxor antiferroelectric (1− x)NaNbO 3−x (0.55BiFeO 3 -0.45SrTiO 3 ) ceramics were elaborately designed and systematically explored. With the help of composition regulation, the ceramics not only exhibited a stable antiferroelectric phase but also underwent a structural transformation from an antiferroelectric P (Pbma) phase to R (Pnma) phase, as confirmed by the temperature-dependent dielectric constants, Raman spectra, X-ray diffraction (XRD) refinement, pinched polarization-electric field (P−E) curves, and four-peak current-electric field (I−E) curves. In addition, the relaxor characteristic was demonstrated by the diffuse dielectric peaks, slim P−E curves, flattened Raman peaks, and I−E curves. Consequently, novel relaxor antiferroelectric ceramics were successfully obtained, which simultaneously revealed the features of relaxor and antiferroelectricity. Specifically, the E b was significantly improved because of the reduced grain size, small sample thickness, exceptionally low dielectric loss, and a moderate dielectric constant. Finally, the sample with x = 0.12 showed an ultrahigh W rec value of 16.2 J/cm 3 and satisfactory η of 82.3% at 97 kV/mm, outperforming most state-of-the-art counterparts. Furthermore, the ceramic also exhibited a large current density (C D ) of 1268.4 A/cm 2 and power density (P D ) of 177.6 MW/cm 3 at 28 kV/mm, offering prospective applications in high-power capacitors. This work not only achieved outstanding comprehensive energy storage performance in sodium niobate-based ceramics by modulating the antiferroelectric structure but also provided a feasible route to developing high-performance dielectric capacitors from the viewpoint of structure−property relationship.