Surface composites are viable choices for various applications in the aerospace and automotive industries. Friction Stir Processing (FSP) is a promising method for fabricating surface composites. Aluminum Hybrid Surface Composites (AHSC) are fabricated using the FSP to strengthen a hybrid mixture prepared with equal parts of Boron carbide (B4C), Silicon Carbide (SiC), and Calcium Carbonate (CaCO3) particles. Different hybrid reinforcement weight percentages (reinforcement content of 5% (T1), 10% (T2), and 15% (T3)) were used in fabricating AHSC samples. Furthermore, different mechanical tests were performed on hybrid surface composite samples with different weight percentages of the reinforcements. Dry sliding wear assessments were performed in standard pin-on-disc apparatus as per ASTM G99 guidelines to estimate wear rates. The presence of reinforcement contents and dislocation behavior was investigated using Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) studies. The results indicated that the Ultimate Tensile Strength (UTS) of sample T3 exhibited 62.63% and 15.17% higher than that of samples T1 and T2, respectively, while the Elongation (%) of T3 exhibited 38.46% and 15.38% lower than that of samples T1 and T2, respectively. Moreover, it was found that the hardness of sample T3 increased in the stir zone compared to samples T1 and T2, owing to its higher brittle response. The higher brittle response of sample T3 compared to samples T1 and T2 was confirmed by the higher value of Young’s modulus and the lower value of Elongation (%).