This paper proposes a non-unity power factor current optimization strategy for three-phase Vienna rectifiers to address current distortion caused by nonsynthetic voltage vectors, especially during current zero-crossing interval under DC-link voltage imbalance, non-unity power factor, and high modulation index conditions. The proposed method minimizes current zero-crossing distortion, improves voltage utilization, and effectively suppresses neutral-point current disturbances. Experimental results from a 2.5 kW prototype verify its superiority over conventional zero-sequence compensation strategies under non-unity power factor and DC-link voltage imbalance.