Material properties of PVDF-TrFE related to dipole alignment and crystallinity, such as surface potential, polarization direction, piezoelectric coefficient, and remnant polarization, have been systematically examined to explain the improvement in the piezoelectric properties of PVDF-TrFE formed at a high spin-coating speed. The correlations between the distribution of the dipole moment vector and the degree of crystallinity were studied as a function of strain rate using a computational molecular dynamic simulation.