Due to its superior high discharge capacity and cycling stability, single-crystal LiNi0.6Co0.2Mn0.2O2 cathode materials are rapidly gaining traction in the realm of electric vehicle power batteries. Nevertheless, the deterioration of surface structure in single-crystal LiNi1−x−yCoxMnyO2 cathode materials is further exacerbated when operating at higher cutoff voltages (exceeding 4.5 V). In this work, a unique single-crystal LiNi0.6Co0.2Mn0.2O2 with ZnO and AlPO4 dual-coating modification has been synthesized. The similar crystal structure of ZnO and NCM results in a more compact coating, while the incorporation of AlPO4 enhances both the electronic conductivity (through the formation of conductive oxide Al-doped ZnO) and lithium-ion conductivity (via the formation of Li3PO4) within the coating. The coated SC-NCM cathode material exhibits excellent electrochemical performance even when operated at a higher cutoff voltage of 4.5 V. After 100 cycles (1 C, 2.75–4.5 V), the capacity retention for the ZnO and AlPO4 coated SC-NCM sample reaches 91.2%, significantly surpassing that of the pristine samples (40.0%). Specifically, it exhibited an outstanding rate property, maintaining a discharge capacity of 150.8 mA h g−1 at 8 C. The exceptional electrochemical properties can be attributed to the distinctive coating layer, which serves not only as a physical barrier to mitigate electrolyte side reactions but also facilitates rapid conduction of electrons and lithium ions.