Metal-organic chemical vapour deposition (MOCVD) is a key technique for fabricating GaN thin film structures for light-emitting and semiconductor laser diodes. Film uniformity is an important index to measure equipment performance and chip processes. This paper introduces a method to improve the quality of thin films by optimizing the rotation speed of different substrates of a model consisting of a planetary with seven 6-inch wafers for the planetary GaN-MOCVD. A numerical solution to the transient state at low pressure is obtained using computational fluid dynamics. To evaluate the role of the different zone speeds on the growth uniformity, single factor analysis is introduced. The results show that the growth rate and uniformity are strongly related to the rotational speed. Next, a response surface model was constructed by using the variables and the corresponding simulation results. The optimized combination of the matching of different speeds is also proposed as a useful reference for applications in industry, obtained by a response surface model and genetic algorithm with a balance between the growth rate and the growth uniformity. This method can save time, and the optimization can obtain the most uniform and highest thin film quality.