As well known, the relaxor dielectric is characterized by high energy storage efficiency (ƞ), while high recoverable energy storage density (Wrec) can be achieved by anti-ferroelectric ceramics. Herein, our approach is to find a relaxor – anti-ferroelectric coexistence phases of (Bi0.5Na0.5)TiO3 – BaTiO3 ceramics for achieving high performance of energy storage and energy harvesting as well. Therefore, [(0.9-x)( Bi0.5Na0.5)TiO3 – xSrTiO3 – 0.1BaTiO3] (abbreviation ((0.9-x)BNT – x ST –0.1BT) (0.0 ≤ x ≤ 0.4) were synthesis via solid-state reaction route in air. The tolerance factor (τ) increased from 0.9901 to 0.9998 when ST-content increased from 0.0 to 0.4 indicate increase the crystal lattice symmetry. The FT-IR de-convolution vibration modes shown the TiO6 octahedra exhibit two peaks at ~ 550 and 650 cm-1 indicate present coexistence phases of crystal structure. Ferroelectric to relaxor phase crossover has been detected by addition of ST with present anti-ferroelectric phase in particular dopant of ST = 0.2. The increasing into the diffused phase transition (γ) is signified to enhancement the relaxor degree of BNT-BT at high content of ST. The rapidly suppression of remnant polarization (Pr) at high content of ST due to substitute iso-valence (Sr2+) by tri-valence (Bi3+) and mono-valence (Na1+). Ultrahigh Wrec = 1.13 J/cm3 with excellent ƞ = 92.62% were obtained at ST=0.3 at low electric field (E=110 kV/cm). Remarkable response of strain with high converse piezoelectric coefficient (d33* = 390.47pm/V) at ST=0.2 was obtained due to decreasing the non-revisable 180o domain switching. Based on the obtained results, the addition of ST into BNT-BT ceramics can provide a head start in the implementation of ceramic capacitors for potential effective into energy harvesting and energy storage applications.