This study is dedicated to the enhancement of electrospun polyacrylonitrile (PAN) nanofiber membranes for their application in membrane bioreactor (MBR) processes. The improvement is achieved through the incorporation of graphitic carbon nitride nanotubes/carbon dots (g-C3N4 NT/CDs) and subsequent heat post-treatments at varying temperatures. Notably, the hot-pressing methodology effectively mitigates surface roughness and significantly reduces issues related to peeling during nanofiber experimentation. Our results demonstrate that the introduction of 0.5 wt% of g-C3N4 NT/CDs leads to a substantial enhancement in water flux. In particular, nanocomposite membranes subjected to hot-pressing at 90 °C for 10 min exhibited an impressive flux recovery ratio (FRR) of 70%. Furthermore, the heat-treated nanocomposite membranes exhibited remarkable antifouling properties and significantly reduced fouling rates when compared to their heat-treated bare counterparts. This study underscores the noteworthy potential of g-C3N4 NT/CDs-modified PAN nanofiber membranes to substantially elevate MBR performance, firmly positioning them as highly promising candidates for critical applications in the domains of water and wastewater treatment. However, it is imperative to underscore that the existing written material necessitates a comprehensive overhaul to align with the provided structural framework.