Grain　size　shows　significant　influence　on　electrical　properties　of　piezoceramics.　However,　there　are　few　works　to　investigate　the　grain　size　effects　in　high-performance　and　large-grain　piezoceramics　and　uncover　the　structure　origin.　In　this　work,　large　grain　size　from　~53　to　~92　µm　was　achieved　in　a　high-performance　BaTiO3　(BT)-based　ceramic　via　tuning　sintering　conditions.　With　grain　size　increasing,　the　ceramics　exhibit　same　multiphase　coexistence　state,　similar　phase　transition　temperature,　upward　TC　dielectric　peaks　and　reduced　diffuseness　degree.　Because　of　the　larger　and　more　complex　non-180°　domains　within　bigger　grains,　the　improvement　in　remnant　polarization　(Pr),　coercive　field　and　negative　strain　were　observed　in　bigger-grain　ceramics.　The　elevated　Pr　finally　leads　to　the　piezoelectric　coefficient　d33　increasing　from　500　to　650　pC/N.　However,　too　large　grains　may　cause　the　reduced　strain　due　to　the　high　remnant　strain　in　first　cycle.　Therefore,　big　grain　size　is　conducive　to　achieve　high　piezoelectricity　while　moderate　grain　size　can　facilitate　strain　response　in　high-performance　ceramics　with　large　grains,　which　is　quite　different　with　pure　BT　ceramic.　This　work　presents　insights　into　the　grain　size　effects　and　affords　guides　to　further　optimize　electrical　properties　in　high-performance　piezoceramics　with　large　grains.　©　2022　Elsevier　Ltd