Multiferroic nanocomposites, consisting of branched, ferrimagnetic CoFe2O4 filaments and large protruding PbTiO3 particles embedded in a piezoelectric PbTiO3 matrix, have been fabricated by co-deposition using metalorganic chemical vapor deposition. Branched CoFe2O4 filaments reduce the CoFe2O4/PbTiO3 interfacial strain and induce a perpendicular magnetic anisotropy. Three-dimensional characterizations reveal that in addition to the c-domain, grains with a second orientation in PbTiO3 particles contribute to an additional four apparent variants of polarization. In contrast, the PbTiO3 matrix exhibits only c-domain polarization with a smaller magnitude. The smaller piezoresponse results from the constraints imposed by the branched CoFe2O4 filaments. Three-dimensional microstructure and property analysis provide a comprehensive insight on the structure-property relationship of multiferroic nanocomposites grown by metalorganic chemical vapor deposition.