In this work, wool fabrics were treated in a corona discharge machine at three different corona intensities and at four fabric speeds. The corona-treated fabrics were subsequently treated with a fiber reactive quaternary ammonium compound, 2,3-epoxypropyltrimethylammonium chloride (EPTAC). The electrostatic propensity, tensile strength, wettability, and surface morphologies of the treated fabrics were assessed. The surfaces of modified wool fabrics were characterized by ATR-FTIR and FT-Raman spectroscopies. It was found that corona treatment decreased the electrostatic propensity only to certain levels, but a significant decrease in corona intensity and an increase in hydrophilicity were observed for the corona-treated fabrics further treated with EPTAC. The tensile strength of the corona in combination with EPTAC-treated fabrics considerably increased over the control fabric, but only small differences in tensile strength were observed for the various corona treatments. ATR-FTIR and FT-Raman spectroscopic results confirmed that EPTAC covalently bonded to the wool fiber surface.