The rapid growth in textile industries has led to a significant discharge of dyed water into water sources, posing severe threats to human and environmental health. Methylene blue (MB), crucial for medical diagnostics and dyeing, requires effective removal due to its toxicological and environmental hazards, persisting above 1 ppm in aqueous solutions at ambient temperatures. Reclaiming cellulose acetate not only heralds a sustainable approach to water reclamation but also amalgamates natural purification with technological advancements. The study utilized reclaimed cellulose acetate to fabricate electrospun nanofibers and bead adsorbents using Ti3C2Tx and surface‐modified Ti3C2Tx via liquid‐state microwaving. The research investigated surface chemistry, morphology, and the impact of adsorption conditions on MB adsorption, revealing enhanced uptake capacities from 45% to 93% for nanofibers and 40%–80% for beads at 25°C after 2 and 3 h, respectively. Adsorption followed PSO kinetics and Langmuir isotherms, with thermodynamic analysis indicating an endothermic, spontaneous physisorption process with ΔH and ΔS values obtained 0.008–31.33 kJ·mol−1 and 11.95–116.38 J·mol−1·K−1. Furthermore, the CA‐surface‐modified Ti3C2Tx composite demonstrated significant photocatalytic activity, achieving 96% degradation efficiency compared to Ti3C2Tx alone. The biodegradation assay under natural conditions using an in‐house degradation slurry showed 20%–58% degradation of the spent adsorbents over 120 days.