Atmospheric pressure plasma treatment using oxygen gas was applied to wool fibrous materials. The plasma-treated fibrous materials were characterised using advanced instrumental techniques including scanning electron microscopy and X-ray photoelectron spectroscopy. They were also tested for performance properties including tensile and tearing strength as well as change in yellowness using international standard testing methods. Wettability analysis was conducted to study the surface area and surface energy of the plasma-treated fibrous materials. Surface modification regarding the enhancement of their adhesion to other substance, i.e. microcapsule treatment, was investigated.