The origins of enhanced piezoelectric coupling along nonpolar crystallographic directions in ferroelectric BaTiO3 are investigated using in situ neutron spectroscopy. It is observed that an electric field applied away from the equilibrium polarization direction causes changes in the phonon spectra that lead to an increase in the interaction between the transverse acoustic and transverse optic branches (TA-TO) near the Brillouin zone center. This provides a direct lattice dynamics mechanism for enhanced electromechanical coupling, and could act as a guide for designing improved piezoelectric materials. ; Comment: 16 pages, 4 figures