Piezocomposites　composed　of　piezoelectric　inorganic　particles　dispersed　in　a　flexible　polymer　have　emerged　as　promising　materials　for　flexible　energy　harvesters　and　sensors.　In　this　work,　to　overcome　the　inefficient　stress　transfer　capability　in　flexible　piezocomposites　for　energy　harvester,　KNbO3　(KN)　particles　prepared　by　conventional　solid　oxide　process　were　aligned　to　form　chain-distributed　particles　in　polydimethylsiloxane　(PDMS)　matrix　by　dielectrophoresis.　The　composite　with　8　vol.-%　KN　has　peak　open　circuit　voltage　of　6.3　V　and　short-circuit　current　of　0.82　mu　A　under　an　applied　force　of　7　N,　which　are　significantly　improved　in　compared　with　the　sample　with　piezoelectric　particles　randomly　dispersed.　Hugely　enhanced　stress-transfer　capability　of　the　aligned　composite　plays　a　key　role　in　achieving　large　piezoelectric　response.　This　work　provides　a　promising　material　candidate　for　high　performance　flexible　energy　harvester.