The field of supercapacitors consistently focuses on research and challenges to improve energy efficiency, capacitance, flexibility, and stability. Low-cost laser-induced graphene (LIG) offers a promising alternative to commercially available graphene for next-generation wearable and portable devices, thanks to its remarkable specific surface area, excellent mechanical flexibility, and exceptional electrical properties. We report on the development of LIG-based flexible supercapacitors with optimized geometries, which demonstrate high capacitance and energy density while maintaining flexibility and stability. Three-dimensional porous graphene films were synthesized, and devices with optimized parameters were fabricated and tested. One type of device utilized LIG, while two other types were fabricated on LIG by coating multi-walled carbon nanotubes (MWCNT) at varying concentrations. Characterization techniques, including scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray diffraction (XRD), Raman spectroscopy, and voltammetry, were employed to analyze the fabricated devices. AFM analysis revealed a surface roughness of 2.03 µm for LIG due to laser treatment. SEM images displayed compact, dense, and porous surface morphology. XRD analysis confirmed the presence of graphene and graphene oxide, which was further supported by energy-dispersive X-ray spectroscopy (EDX) data. Raman spectroscopy indicated that the fabricated samples exhibited distinct D and G bands at 1362 cm–1 and 1579 cm–1, respectively. Cyclic voltammetry (CV) results showed that LIG's capacitance, power density, and energy density were 6.09 mF cm–2, 0.199 mW cm–2, and 3.38 µWh cm–2, respectively, at a current density of 0.2 mA cm–2. The LIG-MWCNT coated electrode exhibited a higher energy density of 6.05 µWh cm–2 and an areal-specific capacitance of 51.975 mF cm–2 compared to the LIG-based devices. The fabricated device has potential applications in smart electronics, nanorobotics, microelectromechanical systems (MEMS), and wearable and portable electronics.