Increasing energy demands and growing environmental concerns regarding the consumption of fossil fuels are important motivations for the development of clean and sustainable energy sources. A triboelectric nanogenerator (TENG) is a promising energy technology that harnesses mechanical energy from the ambient environment by converting it into electrical energy. In this work, the enhancement of the energy conversion performance of a natural rubber (NR)-based TENG has been proposed by using modified activated carbon (AC). The effect of surface modification techniques, including acid treatments and plasma treatment for AC material on TENG performance, are investigated. The TENG fabricated from the NR incorporated with the modified AC using N2 plasma showed superior electrical output performance, which was attributed to the modification by N2 plasma introducing changes in the surface chemistry of AC, leading to the improved dielectric property of the NR-AC composite, which contributes to the enhanced triboelectric charge density. The highest power density of 2.65 mW/m2 was obtained from the NR-AC (N2 plasma-treated) TENG. This research provides a key insight into the modification of AC for the development of TENG with high energy conversion performance that could be useful for other future applications such as PM2.5 removal or CO2 capture.