Superparaelectrics are considered promising candidate materials for achieving superior energy storage capabilities. However, due to the complicated local structural design, simultaneously achieving high recoverable energy density (W_rec) and energy storage efficiency (η) under high electric fields remains a challenge in bulk superparaelectrics. Here, we propose utilizing entropy engineering to disrupt long-range ferroic orders into local polymorphic distortion disorder with multiple BO₆ tilt types and diverse heterogeneous polarization configurations. This strategy reduces the switching barriers, thereby facilitating the emergence of superparaelectric behaviors with ideal polarization forms. Furthermore, it enables high polarization response, negligible remnant polarization, delayed polarization saturation, and enhanced breakdown electric fields (E_b) in high-entropy superparaelectrics. Consequently, an extraordinary W_rec of 15.48 J cm^–3 and an ultrahigh η of 90.02% are achieved at a high E_b of 710 kV cm^–1, surpassing the comprehensive energy storage performance of previously reported bulk superparaelectrics. This work demonstrates that entropy engineering is a viable strategy for designing high-performance superparaelectrics.

Research on doping modification of ZnTiO₃ ceramics to enhance microwave dielectric properties has been hindered by poor performance, unclear structure-function mechanisms. To expand the applicability of ZnTiO₃ ceramics, this study explores Zn_1–xLi_2xTiO₃ (0 ≤ x ≤ 1) ceramics using a phase engineering strategy. Our findings reveal that the introduction of Li⁺ into the ZnTiO₃ system initiates a multiple phase transition, starting at x = 0.1. Initially, ilmenite ZnTiO₃ transforms into a cubic ordered spinel phase (space group P4332). Subsequently, a transition to a disordered spinel phase (space group Fd-3m) occurs at x = 0.5, culminating in the formation of a monoclinic rock salt-structured Li₂TiO₃ phase. Significantly, two sets of ceramics with near-zero temperature coefficients of resonance frequency (τ_f) were obtained at x = 0.1 and 0.75. Moreover, the quality factor (Q×f) demonstrated a 4.4-fold increase compared to that of ZnTiO₃ ceramics at x = 0.25 (105,013 GHz). Additionally, it was observed that the Ti⁴⁺ polarization in Zn_1–xLi_2xTiO₃ ceramics had been underestimated by 11.3-13.3%, causing the measured dielectric constant (ε_r) exceeding the theoretical dielectric constant (ε_th). The ionic polarizability of Ti⁴⁺ was adjusted to stabilize around 3.29 ų. Evaluation using multiple methods, including Phillips–Van Vechten–Levine theory, Raman vibrational mode analysis, bond valence, bond energy theory, and octahedral distortion, confirms that the Ti-O bonds within the octahedron predominantly affect ε_r, the increasing lattice energy (U) contributes to the enhancement of Q×f, and the strengthened Li-O bond energy effectively regulates τ_f.