Oxide dielectrics, such as HfO, AlO, etc, are widely used to improve the performance of 2D semiconductors in electronic devices. However, future low-power electronic devices need a higher dielectric constant (κ) to reduce the leakage current, and these super-high-κ materials are challenging to produce on wafer-scale. Here, the preparation of wafer-scale (Ga, Cu) co-doping ZnO films is reported with super-high dielectric constant (κ > 50) and good homogeneity by a pulsed laser deposition method. By regulating the (Ga, Cu) co-doping concentration, the dielectric constants can range from 9 to 207. In addition, the performance of SnS field-effect transistor reveals that the high-κ AlO/GCZO gate dielectric stack is suitable for 2D electronic devices. This GCZO dielectric films not only show higher κ than other conventional dielectrics in terms of compatibility to CMOS processes, but also keep their comparative advantages in the fabrication of high-performance electronic devices over conventional dielectrics.