Previous　piezoelectric　energy　harvesters　usually　employ　flexible　composite　films　based　on　nanosized　piezoelectric　fillers.　In　this　work,　large　piezoelectric　particles　with　micron　sizes　were　used　to　prepare　high-performance　piezoelectric　composite　films　after　forming　a　polydopamine　(PDA)　shell　on　the　particles　and　introducing　them　into　a　flexible　polydimethylsiloxane　(PDMS)　matrix.　The　large　piezoelectric　fillers　contribute　to　a　high　property　but　are　difficult　to　achieve　a　homogeneous　distribution.　The　PDA　shell　can　afford　tight　interface　bonding　between　piezoelectric　fillers　and　the　matrix　and　lead　to　the　homogeneous　distribution　of　large　fillers　even　if　the　filler　content　is　＞50　wt　%.　The　validity　was　verified　in　different　piezoelectric　energy　harvesters　based　on　large-particle　Pb(Zr,　Ti)O3/PDMS　and　(Ba,　Ca)(Ti,　Zr)O3/PDMS　composite　films.　These　composite　films　show　superior　mechanical,　ferroelectric,　piezoelectric,　and　energy　harvesting　performances　after　PDA　modification.　A　high　output　current　of　∼250-390　nA　can　be　obtained　in　relevant　piezoelectric　harvesters　under　a　low　stimulating　force　of　2-10　N.　The　obtained　current　under　unit　force　exceeds　the　results　of　most　previous　piezoelectric　energy　harvesters.　This　work　affords　a　general　strategy　to　obtain　high-performance　piezoelectric　energy　harvesters　based　on　large　piezoelectric　fillers　and　PDA　modification.　©　2024　American　Chemical　Society