Wool is a natural composite fiber, with keratin and keratin-associated proteins as the key molecular components. The outermost surface of wool fibers comprises a hydrophobic lipid layer that can lead to unsatisfactory processing and properties of fabric products. In this study, molecular sieve 5A, a Na' and Ca2+ exchanged type A zeolite with a 1:1 Si:Al ratio was integrated onto the surface of wool using 3-mercaptopropyl trimethoxy silane. The resultant surface morphology, hydrophilicity and mechanical performance of the treated wool fabrics were then evaluated. Notably, the surface hydrophilicity of wool was observed to increase dramatically. When wool was treated with a dispersion of 2 wt% acetic acid, 2.5 wt% zeolite and 0.3 wt% or more silane, the water contact angle was observed to decrease from an average value of 148 degrees to 0 degrees over a period of approximately 30s. Scanning electron microscopic imaging indicated good coverage of the wool surface with zeolite particles, with infrared spectroscopic evaluation indicating strong bonding of the dealuminated zeolite to wool keratins. This application of zeolite showed no adverse effects on the tensile and other mechanical properties of the fabric. This study indicates that zeolite-based treatment is a potentially efficient approach to increasing the surface hydrophilicity and modifying other key surface properties of wool and wool fabrics. (C) 2013 Elsevier B.V. All rights reserved.