Magnetoelectric　coupling　properties　are　limited　to　the　substrate　clamping　effect　in　traditional　ferroelectric/ferromagnetic　heterostructures.　Here,　Fe3O4/BaTiO3　nanopillar　composites　are　successfully　constructed.　The　well-ordered　BaTiO3　nanopillar　arrays　are　prepared　through　template-assisted　pulsed　laser　deposition.　The　Fe3O4　layer　is　coated　on　BaTiO3　nanopillar　arrays　by　atomic　layer　deposition.　The　nanopillar　arrays　and　heterostructure　are　confirmed　by　scanning　electron　microscopy　and　transmission　electron　microscopy.　A　large　thermally　driven　magnetoelectric　coupling　coefficient　of　395　Oe　degrees　C-1　near　the　phase　transition　of　BaTiO3　(orthorhombic　to　rhombohedral)　is　obtained,　indicating　a　strong　strain-induced　magnetoelectric　coupling　effect.　The　enhanced　magnetoelectric　coupling　effect　originated　from　the　reduced　substrate　clamping　effect　and　increased　the　interface　area　in　nanopillar　structures.　This　work　opens　a　door　toward　cutting-edge　potential　applications　in　spintronic　devices.