Piezoelectric　energy　harvesters　(PEHs)　with　piezoceramics　as　the　core　can　convert　low-frequency　vibration　energy　that　is　ubiquitous　in　the　environment　into　electrical　energy　and　are　at　the　frontier　of　research　in　the　field　of　energy.　The　high　piezoelectric　charge　coefficient　(d)　together　with　the　large　piezoelectric　voltage　coefficient　(g)　are　essential　for　enhancing　the　energy　harvesting　performances　of　PEHs　working　on　a　nonresonant　state.　However,　conventional　doping　and　solid　solution　design　strategies　lead　to　the　same　increase　or　decrease　trend　of　d　and　dielectric　permittivity　ε,　making　it　difficult　to　obtain　a　high　g　value　because　g　=　d/ε.　Herein,　exceptionally　well-balanced　performances　of　high　d　and　large　g　are　achieved　simultaneously　in　modified　Pb(Zr,　Ti)O3(PZT)-based　ceramics　via　a　multiscale　heterogeneity　strategy,　which　involves　coordination　among　the　defect　dipole,　hierarchical　domain,　and　composite.　The　electromechanical　parameters　of　the　optimal　specimen　are　not　only　superior　to　those　of　many　state-of-the-art　commercial　counterparts　but　also　exhibit　good　thermal　stability.　Most　importantly,　the　assembled　PEH　with　the　optimal　specimen　shows　excellent　variable　temperature　power　generation　characteristics.　This　work　provides　a　paradigm　for　building　PEH　material　through　a　multiscale　heterogeneity　strategy,　expected　to　benefit　a　wide　range　of　electromechanical　coupling　materials.