Nowadays, the environmental challenges associated with plastics are becoming increasingly prominent, making the exploitation of alternatives to landfill disposal a pressing concern. Particularly, polyvinyl chloride (PVC), characterized by its high chlorine content, poses a major environmental risk during degradation. Furthermore, PVC recycling and recovery present considerable challenges. This study aims to optimize the PVC pyrolysis valorization process to produce effective adsorbents for removing contaminants from gaseous effluents, especially COsub.2. For this purpose, PVC waste was pyrolyzed under varied conditions, and the resulting solid fraction was subjected to a series of chemical and physical activations by means of hydroxides (NaOH and KOH) and nitrogen. Characterization of the PVC-based activated carbons was carried out using surface morphology (SEM), Nsub.2 adsorption/desorption, elemental analysis, and FTIR, and their capacity to capture COsub.2 was assessed. Finally, neuro-fuzzy models were developed for the optimization of the valorization technique. The resulting activated carbons exhibited excellent COsub.2 adsorption capabilities, particularly those activated with KOH. Optimal activation conditions include activations at 840 °C with NaOH at a ratio of 0.66 and at 760 °C using either NaOH or KOH with ratios below 0.4. Activations under these experimental conditions resulted in a significant increase in the adsorption capacity, of up to 25%, in the resulting samples.