Traditional supercapacitors are cumbersome and need separate enclosures, which add weight and reduce space efficiency. In contrast, structural supercapacitors combine energy storage with load-bearing materials, optimizing space and weight for automotive and aerospace applications. This study investigates the synthesis of SmVO₄-MoS₂ and SmVO₄-MoS₂-CNT nanocomposites, focusing on optimizing CNT concentration in SmVO₄-MoS₂-CNT for high-performance supercapacitors. The optimal concentration of SmVO₄-MoS₂-CNT is identified and used to fabricate structural supercapacitor devices via the vacuum-assisted resin transfer molding (VARTM) technique. The results indicate that the specific capacitance of Sm-Mo-C5, using a three-electrode system, reached 1.01 F cm⁻² at a current density of 2.187 mA cm⁻². The performance improvement is attributed to the synergistic interaction among SmVO₄, MoS₂, and CNTs, collectively enhancing conductivity and active site availability. The practical application of this study is demonstrated by synthesizing Sm-Mo-C5 on woven carbon fiber (WCF) and subsequently fabricating a structural supercapacitor device (SSD) using the VARTM. The SSD, produced via VARTM, exhibited a specific capacitance of 0.287 F cm⁻² at a current density of 2 A cm⁻². The device showcased exceptional cyclic stability, maintaining 72.5% of its initial capacitance after 50,000 charge-discharge cycles. Additionally, it achieved a maximum energy density of 79.86 Wh kg⁻¹ at a power density of 1017.69 W kg⁻¹.