In this paper, optimization of the fabrication parameters of an aluminum surface composite with respect to tensile strength and tool wear rate is reported. The surface layer was reinforced with SiC particles to improve the tribological properties of AA-5052. The Taguchi design with orthogonal array L8 was used for the experimental design, which included three processing parameters: the number of passes, rotational speed, and traversal speed. The experiment used optimal fabrication parameter searching to produce a multi-response prediction of both the tensile strength and tool wear rate. The experimental result was determined by grey relational analysis for multi-performance characteristics. Afterward, the prediction result of the optimal fabrication parameters was confirmed by repeated experiments to confirm the selection of optimal process parameters. The results revealed that the optimal fabrication parameters for multi-performance characteristics are two passes, rotational speed of 1000 revolutions per minute (RPM), and traversal speed of 30 mm/min (condition N2R1T2). These showed high tensile strength (229.90 MPa), low tool wear rate (0.0851), and a uniform distribution of SiC particles in the matrix. In addition, grey relational analysis showed that the parameter priority was 51.68% for rotational speed (the most significant process parameter), 36.18% for transversal speed, and 7.05% for the number of passes. Therefore, the grey-based orthogonal array Taguchi method can optimize multi-performance characteristics through the setting of process parameters for friction stir processing of an aluminum surface composite.