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From the environmental point of view, there is high demand for the preparation of polymeric materials for various applications from renewable and/or waste sources. New lignin-based spun fibers were produced, characterized, and probed for use in methylene blue (MB) dye removal in this study. The lignin was extracted from palm fronds (PF) and banana bunch (BB) feedstock using catalytic organosolv treatment. Different polymer concentrations of either a plasticized blend of renewable polymers such as polylactic acid/polyhydroxybutyrate blend (PLA-PHB-ATBC) or polyethylene terephthalate (PET) as a potential waste material were used as matrices to generate lignin-based fibers by the electrospinning technique. The samples with the best fiber morphologies were further modified after iodine handling to ameliorate and expedite the thermostabilization process. To investigate the adsorption of MB dye from aqueous solution, two approaches of fiber modification were utilized. First, electrospun fibers were carbonized at 500 °C with aim of generating lignin-based carbon fibers with a smooth appearance. The second method used an in situ oxidative chemical polymerization of m-toluidine monomer to modify electrospun fibers, which were then nominated by hybrid composites. SEM, TGA, FT-IR, BET, elemental analysis, and tensile measurements were employed to evaluate the composition, morphology, and characteristics of manufactured fibers. The hybrid composite formed from an OBBL/PET fiber mat has been shown to be a promising adsorbent material with a capacity of 9 mg/g for MB dye removal.