To　build　piezoceramics　with　high　transduction　coefficient　(d(33)　x　g(33))　is　the　key　to　improve　the　power　generation　capability　of　piezoelectric　energy　harvester.　Here,　a　new　targeted　doping　strategy　has　been　proposed　to　significantly　increase　the　energy　density　of　piezoceramics.　Taking　the　modification　of　0.2Pb(Zn1/3Nb2/3)O-3-0.8Pb(Zr0.5Ti0.5)O-3　(PZN-PZT)　as　an　example,　dual　functions　can　be　achieved　by　introducing　appropriate　amount　of　target-doped　(Zn0.1Ni0.9)　TiO3　(ZTN9)　based　on　its　pyrolysis　characteristics.　On　the　one　hand,　Ni2+　ions　enter　the　perovskite　matrix　to　replace　Zn2+　ions　to　form　equivalent　doping;　on　the　other　hand,　it　induces　the　formation　of　0-3　ZnO/perovskite　composite　structure,　and　both　of　which　promote　the　large　increase　in　d(33)　x　g(33)　due　to　the　changes　in　the　domain　configuration　are　more　conducive　to　the　ferro-/piezoelectricity.　In　all　compositions,　0.67　mol%　ZTN9　added　specimen　has　a　maximum　value　(12　433　x　10(-1)5　m(2)/N)　of　the　d(33)　x　g(33).　The　cantilever　piezoelectric　energy　harvester　fabricated　with　this　material　generates　up　to　4.50　mu　W/mm(3)　of　power　density　at　1　g　acceleration,　which　is　capable　of　quickly　charging　a　47　mu　F　electrolytic　capacitor　and　then　lit　135　parallel-connected　commercial　blue　light-emitting　diodes　(LEDs),　showing　its　important　application　in　implementing　self-powered　microsensors.