This work aims to study the mechanical theory and finite element method (FEM) prediction method for shot peening deformation of aerospace arc-shaped frame, and establish the specification of shot peening process to provide guidance for shot peening in the domestic aviation industry. Firstly, several groups of random shot impact simulations with different shot speeds were carried out by ABAQUS, and a shot peening induced stress database related to the average shot speed was created. Based on this, theoretical prediction and finite element simulation of shot peening deformation of arc-shaped frame were carried out; in the ABAQUS environment, a plug-in for quickly simulating the shot peening deformation of arc-shaped frame under different peening parameters was developed. By using this plug-in, all operations could be done automatically in the fore treatments of ABAQUS for various types of arc-shaped frames, and theoretical and simulation results could be given at the same time. Based on the above research, a process specification for quickly determining the shot peening parameters of various arc-shaped frames was developed. For specific aerospace arc-shaped frame, the theoretical maximum deformation was 1.25 mm; the maximum deformation calculated by FEM was 1.13 mm; and the experimental result was 1.8 mm under the same shot parameters. Combined with calculation prediction and process specification, the shot peening area and parameters were determined; and the final deformation of the arc-shaped frame was 0.15 mm, which met the accuracy requirements. The validity of the calculation prediction and specification was verified. Through the analysis, theoretical prediction method and FEM can quickly and accurately predict the results of shot peening deformation of arc-shaped frame. This study is of engineering value for the quick simulation and theoretical prediction of the shot peening deformation results of the arc-shaped frame in the domestic aviation industry.