AbstractEnvironmental concerns and the over‐exploitation of natural resources have driven the search for eco‐friendly materials. Agro/industrial waste, often discarded, can be repurposed as fillers in biocomposites. However, bio‐fibers present challenges such as poor compatibility, high moisture absorption, and variable mechanical properties. This study examines various fiber surface modification techniques, including NaOH, silane, alkali‐silane, and pectinase enzyme treatments on enset fiber (EF) to produce sustainable reinforced poly(lactic acid) (PLA) composites. Untreated EF/PLA composites were fabricated for comparison. Results showed that the applied EF surface treatments, especially using pectinase enzyme, significantly enhanced mechanical, thermal, and thermomechanical properties. Pectinase‐treated EF/PLA composites displayed increased tensile strength by 55.99%, elongation at the break by 39.49%, tensile modulus by 32.59%, impact strength by 51.50%, flexural strength by 51.85%, flexural modulus by 60.90%, and improved thermal stability as compared to untreated composite. Scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR) analyses verified better fiber‐matrix interaction with clarity due to reduced non‐cellulosic components. Pectinase enzyme treatment emerged as the most effective, eco‐friendly method, enhancing the enset fiber's potential in polymer biocomposites, suitable for automotive interiors and packaging industries, reducing synthetic plastic pollution, and utilizing agricultural waste.Highlights Enset fibers were modified by NaOH, silane, NaOH/silane, and pectinase enzyme The modified enset/PLA composites were prepared by compression molding Surface treatments enhanced the enset‐PLA matrix interaction Pectinase‐modified enset/PLA composite showed superior properties Improved properties of enset composites make it ideal for various applications
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