Coir fibers were chemically modified through alkali treatment, and crosslinking with formaldehyde, para-phenylene diamine, phthalic anhydride, and combined crosslinking-cyanoethylation reactions in appropriate solvent and catalyst. The parent and chemically modified coir were characterized by FTIR spectra. The percent moisture regain, tensile strength, and behavior toward some chemical reagents (solubility %) of parent and chemically modified fibers have also been evaluated. The modified fibers showed significant hydrophobicity, improved tensile strength, and good chemical resistance.