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Biocomposites based on poly(L-lactic acid) (PLA) and non-woven jute fabrics (NWJF) were fabricated by sandwiching non-woven jute mat between PLA sheets. First, composites were fabricated with various weight proportions of jute fabric (5, 10, 20, and 30 wt.%) with the PLA matrix, and the effect of fabric loading on their mechanical properties was investigated. Higher mechanical properties were found at 10 wt.% fabric-loaded composite. The results show that the tensile, flexural, and impact strengths were increased by 61.7, 52.3, and 47.2%, respectively, as compared with neat PLA. In the second part, the jute fabrics were chemically treated with NaOH, NaClO2, acrylonitrile, acetic anhydride, KMnO4, diphenylmethane diisocyanate, and benzoyl chloride. The effect of chemical treatment on the mechanical and water absorption properties of NWJF/PLA biocomposites was studied. The mechanical properties of these biocomposites were found to be higher than those of untreated biocomposites. Among all the treatments, the combined alkali-benzoylated-treated fabric composite showed higher mechanical properties. The water absorption properties of these composites were found to be remarkably lower than those of untreated fibers. The interfacial adhesion between the fiber and the matrix was shown to increase with surface modification as revealed by SEM analysis.