Three different silicone polymer systems, such as aminofunctional, epoxyfunctional, and hydrophilic epoxyfunctional silicone polymers, were applied onto plasma pretreated wool fabric to improve the dimensional properties. The results showed that the plasma pretreatment modified the cuticle surface of the wool fiber and increased the reactivity of wool fabric toward silicone polymers. Felting shrinkage of plasma and silicone treated wool fabric was decreased with different level depending on the applied polymer system. Fabric tear strength and hand were adversely affected by plasma treatment, but these properties were favorably restored on polymer application. Therefore, it has been concluded that the combination of plasma and silicone treatments can achieve the improved dimensional stability, and better performance properties of wool fabric. The surface smoothness appearances of treated fabrics were measured using a new evaluation system, which showed good correspondence with the results of KES-FB4 surface tester.