Wool is a naturally occurring composite fiber consisting of keratin and keratin-associated proteins as the key molecular components. The outermost surface of wool comprises a lipid layer that renders the surface hydrophobic, which hinders certain fabric processing steps and moisture management properties of wool fabrics. In this study, Linde Type A (LTA) nano-zeolite (a Na 1 -, Ca 21 -, and K 1 -exchanged type A zeolite) was integrated onto the surface of wool using 3-mercaptopropyl trimethoxy silane as a bridging agent. The resultant surface morphology, hydrophilicity, and mechanical performance of the treated wool fabrics were evaluated. Notably, the surface hydrophilicity of wool increased dramatically. When wool was treated with a dispersion of 1 wt % zeolite and 0.2 wt % silane, the water contact angle decreased from an average value of 1488 to 508 over a period of approximately 5 min. Scanning electron microscopic imaging indicated good coverage of the wool surface with zeolite particles, and infrared spectroscopic evaluation demonstrated strong bonding of the zeolite to wool keratins. The zeolite application showed no adverse effects on the tensile and other mechanical properties of the fabric. This study indicates that zeolite-based treatment is potentially an efficient approach to increasing the surface hydrophilicity and modifying other key surface properties such as softness of wool and wool fabrics. V C 2015Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 42392.