We use molecular dynamics to calculate the structural, elastic, and polar properties of crystalline ferroelectric β -poly(vinylidene fluoride), PVDF (-CH 2 -CF 2 -) n with randomized trifluoroethylene TrFE (-CHF-CF 2 -) n as a function of TrFE content (0-50%) in the temperature range of 0-400 K. There is a very good agreement between the experimentally obtained and the computed values of the lattice parameters, thermal expansion coefficients, elastic constants, polarization, and pyroelectric coefficients. A continuous decrease in Young's modulus with increasing TrFE content was observed and attributed to the increased intramolecular and intermolecular repulsive interactions between fluorine atoms. The computed polarization displayed a similar trend, with the room temperature spontaneous polarization decreasing by 44% from 13.8 µC/cm 2 (pure PVDF) to 7.7 µC/cm 2 [50/50 poly(VDF-co-TrFE)]. Our results show that molecular dynamics can be used as a practical tool to predict the mechanical and polarization-related behavior of ferroelectric poly (VDFco-TrFE). Such an atomistic model can thus serve as a guide for practical applications of this important multifunctional polymer. . Fax:+1 860 486 2981; Tel:+1 860 486 2012 ‡ These authors contributed equally to this work. J o u r n a l N a me , [ y e a r ] , [ v o l . ] , 1-8 | 1