This research introduces a novel upcycling method for transforming cigarette filters—an abundant and persistent environmental waste—into high-performance epoxy composites reinforced with cellulose nanofibers. The innovation lies in extracting cellulose acetate nanofibers from used cigarette butts via a multi-step purification and electrospinning process, followed by their conversion into regenerated cellulose nanofibers through alkaline hydrolysis. This dual-fiber approach allows us to fabricate four distinct epoxy composites, each reinforced by different nanofiber types: recycled cellulose acetate nanofibers, regenerated cellulose nanofibers from recycled cigarette filters, and their commercial counterparts. Notably, this is the first time regenerated nanofibers derived from waste cigarette filters have been utilized for epoxy composite reinforcement, demonstrating a sustainable, high-value use for a major pollutant. Comprehensive characterizations, including FTIR, XRD, SEM, and contact angle measurements, confirmed the successful regeneration of cellulose nanofibers, showing improved hydrophilicity, reduced crystallinity, and uniform nanofiber morphology with diameters between 200 and 300 nm. The innovation further extends to the mechanical performance of these composites: tensile tests revealed that those reinforced with regenerated cellulose nanofibers exhibited superior tensile strength (49.5–53.8 MPa), significantly outperforming both cellulose acetate nanofiber composites (40.1–42.6 MPa) and neat epoxy resin (31.4 MPa). This marked improvement is attributed to enhanced nanofiber dispersion and interfacial adhesion within the epoxy matrix, an essential advancement over traditional composites. In addition, thermal analysis showed that all composites maintained thermal stability in the 300–400 °C range, comparable to commercial alternatives. The regenerated nanofiber-reinforced composites also displayed enhanced optical transparency due to reduced light scattering, making them ideal candidates for applications requiring both mechanical strength and optical clarity. By pioneering the use of cigarette filter waste for fabricating advanced cellulose nanofiber composites, this study presents an eco-friendly approach to addressing environmental pollution while creating sustainable materials with superior mechanical, thermal, and optical properties.