A multiscale regulation strategy has been demonstrated for synthetic energy storage enhancement in a tetragonal tungsten bronze structure ferroelectric. Grain refining and second-phase precipitation (perovskite phase) are introduced in the BaSrTiNb2-xTaxO9 ceramics by regulating the composition and sintering process. Disordered polarization and distribution, chemical inhomogeneity, and insulating boundary layers are achieved to provide the fundamental structural origin of the relaxation characteristic, high breakdown strength, and superior energy storage performance. Thus, an ultrahigh energy storage density of 12.2 J cm−3 with an low energy consumption was achieved at an electric field of 950 kV cm−1. This is the highest known energy storage performance in tetragonal tungsten bronze-based ferroelectric. Notably, this ceramic shows remarkable stability over frequency, temperature, and cycling electric fields. This work brings new material candidates and structure design for developing of energy storage capacitors apart from the predominant perovskite ferroelectric ceramics.