Alternating current poling (ACP) is an effective method to improve the piezoelectric performance of relaxor-PbTiO3 (PT) ferroelectric single crystal. 0.72Pb(Mg1/3Nb2/3)O3-0.28PbTiO3 (PMN-PT) single crystals have been used to fabricate piezoelectric transducers for medical imaging. Up to date, there are no reports about the full matrix material constants of PMN-0.28PT single crystals poled by ACP. Here, we report the complete sets of elastic, dielectric, and piezoelectric properties of [001]-poled PMN-0.28PT single crystals by direct current poling (DCP) and ACP through the resonance method. The results show that [001]-poled rhombohedral PMN-0.28PT single crystals exhibit the enhancement of longitudinal and transverse piezoelectric properties ( d33 ∼ 2000 pC/N, d31 ∼ -1010 pC/N) after ACP. Compared with DCP samples ( d33 ∼ 1660 pC/N, d31 ∼ -780 pC/N), the values of d33 and d31 increase 20% and 29%, respectively. While the d15 value decrease from 110 pC/N for DCP sample to 90 pC/N for ACP sample, showing the decrease in transverse shear piezoelectric properties. In addition, the elastic stiffness coefficients c11 , c12 , c13 , the elastic compliance coefficients s11 , s12 , and the dielectric constants ε11 , ε33 have great change compared with DCP and ACP samples. This variation of the property matrices provides a reference for high-performance piezoelectric device design.