There is a surge in research in the domain of polymer nanocomposite-based triboelectric nanogenerators (TENG), yet, underpinning the influence of embedded nanomaterials, their functionalities, and interaction with polymer functional groups towards controlling the TENG output remains limited, especially in cases involving anisotropic fillers like carbon nanotubes. In this work, we investigate a model comprising amine-modified multiwalled carbon nanotubes and maleic anhydride functionalized liquid rubber for interfacial charge orchestration. We decoded how bidirectional electrical conductivity, charge dispersion, and dielectric properties can synergistically govern the TENG outcome. An empirical mathematical equation was established to correlate the dielectric properties, directional conductivities, and TENG output. The fitted curve demonstrated strong agreement with experimental data. The optimized TENG device, stable over 30,000 cycles, demonstrated an open-circuit voltage of 253.23  V, short-circuit current of 71.13 μA, short-circuit charge of 92.48 nC, and a power density of 7.70 W/m 2, surpassing existing CNT-polymer-based systems. Finally, the TENG devices were utilized to develop a remote that can control the various electronic devices without any internet within the range of ~400 m. This work not only advances material-level insight into anisotropic nanocomposites for TENG but also acts as an enabler for sustainable energy and intelligent device interfacing.