Multiwall carbon nanotubes (MWCNTs) are utilized to resolve low coupling coefficient issue by dispersing MWCNTs in poly(vinylidene fluoride) matrix to create stress reinforcing network, dispersant, and electron conducting functions for barium titanate (BT) nanoparticles. Various BT and MWCNT percentages of nanocomposite film are fabricated by FDM three-dimensional (3D) printing which can simplify the fabrication process as well as lower cost and design flexibility. Increasing MWCNTs and BT particles gradually increase piezoelectric coefficient (d
31) by 0.13 pC/N with 0.4 wt%-MWCNTs/18 wt%-BT. These results provide not only a technique to print piezoelectric nanocomposites but also unique materials combination for sensor application.