The investigation of efficient research approaches to boost the output performance of triboelectric nanogenerators (TENGs) is crucial in extending their practical use in daily life. In this study, a laser-carbonized (LC) MXene/ZiF-67 nanocomposite-based intermediate layer is introduced to achieve outstanding output performance in both contact and non-contact mode (CNM) TENGs. The porous structure of the LC-MXene/ZiF-67 nanocomposite layer contains a high charge density, thereby enabling the surface charges to be conserved for longer periods, and simultaneously increasing the surface potential. Different ratios of MXene/ZiF-67, laser powers, and laser speeds were explored and optimized to improve the output performance of the CNM-TENG. Under optimal conditions, the intermediate and charge generating layer significantly enhanced the contact-TENG output power density of 65 W/m2 at a load resistance of 1.3 MΩ. In addition, the noncontact TENG provided a high charge density of 15.3 µC/m2 and stable output performance at a distance of 2 cm. Finally, demonstrations of the optimized CNM-TENG-based human gait analysis, automobile vehicles, smart robots were presented to enable obstacle detection and human motion alerts, touchless wearable keyboards for security, and self-powered electronic devices. The findings of this study offer an innovative and effective strategy for designing devices with excellent performance for use in self-powered electronic devices and sensing systems.