Pb-based relaxor piezoelectric single crystal composites (PSCCs) have attracted widespread attention for improving the bandwidth and sensitivity performance of acoustic transducers due to their excellent electromechanical and piezoelectric properties. Alternating current polarization (ACP) has been proven as an effective method for enhancing the dielectric and piezoelectric properties of relaxor-PbTiO3 single crystals. Herein, we investigated the effects of the amplitude, frequency, and cycle number of the poling electric field on the piezoelectric and dielectric performances of PSCCs and obtained the optimum poling condition of ACP. Compared with the traditional direct current poling method, both the dielectric permittivity (ε33T/ε0) and piezoelectric coefficient (d33) of the AC-poled PSCCs were both increased by up to 20%. Notably, the ACP PSCC with a volume fraction of 60% exhibited a high d33 of 1610 pC/N, which is superior to values previously reported for PSCCs. This work provides an alternative strategy for enhancing the properties of PSCCs and may contribute to the further development of piezoelectric applications.