This research focused on the characteristics of the AA6061/AA5083 alloy joints which are fabricated by the friction stir welding (FSW) technique. The impact of FSW parameters such as tool tilt angle, pin depth, and tool geometry on the mechanical properties and fractographic characteristics were studied. Ultimate tensile strength (UTS), hardness (HBN), and specific wear rate (SWR) were examined for characterization while fractography analyses were done using scanning electron microscopy. Taguchi-Grey relational analysis (GRA) was employed to execute multicriteria optimization and recognize the best grouping of parameters. The optimized values attained from this analysis were 259.2 MPa for UTS, 94.9 HV for HBN, and 0.0819 m³/Nm for SWR. The analysis of variance (ANOVA) results derived from the GRA revealed that tool geometry exerted the most significant influence (39.79%) on output factors, followed by pin depth (24.90%) and tilt angle (24.26%). To enhance the predictive accuracy of the output responses, an artificial neural network (ANN) model was developed utilizing the Levenberg-Marquardt (LM) algorithm. The optimized ANN architecture, configured as (3–10–3), exhibited robust regression analysis outcomes, showcasing correlation coefficients ( R) of 0.99999, 0.99967, and 0.99994 for the training, validation, and test datasets. The overall R-value, computed at 0.99958, affirmed high conformity between experimental and predicted values.