Significant progress in surface modification techniques has been promoted by the need for novel fabrics with improved functionality and customized qualities. In order to obtain desired qualities such as enhanced wettability, functional characteristics, antimicrobial activity, self-cleaning qualities, flame retardancy, and dye uptake, surface modification in terms of physicochemical techniques is important. This chapter examines the role of physicochemical approaches in changing and functionalizing textile surfaces. It gives a thorough rundown of methods, stressing their fundamental workings, benefits, and drawbacks. These methods include sol–gel procedures, grafting techniques, plasma technologies, and other surface modification techniques. The chapter explores how each surface modification techniques bring change with respect to physical, mechanical, structural, and chemical properties of textile materials. Advancements and challenges for industrial applications and future research are also briefly discussed.