A 1,2,3,4-butanetetracarboxylic acid (BTCA)-sodium hypophosulfite (SHP) wrinkle-resistance system played an important role in improving the wrinkle-resistance properties of cotton fibers. In this study, titanium dioxide (TiO 2 ) was used as a cocatalyst to further enhance the wrinkle-resistance properties of BTCA-SHP-treated cotton fabrics, that is, those treated with (1) 5% BTCA and 10% SHP; (2) 5% BTCA, 10% SHP, and 0.1% TiO 2 ; and (3) 5% BTCA, 10% SHP, and 0.2% TiO 2 . In addition, the effect of plasma as a pretreatment process on the wrinkle-resistance properties of the three treatment systems was also studied. The experimental results reveal that the wrinkle-resistance properties of cotton fibers were improved after different wrinkle-resistance treatments. In addition, the plasma pretreatment further enhanced the wrinkle-resistance treatments to different extents, depending on the process parameters. Scanning electron microscopy images confirmed that such plasma pretreatment conditions imparted the best crosslinking effect on the cotton fibers. However, the wrinkle-resistance-treated cotton specimens had lower tensile strength and tearing strength values compared to the control sample, whereas the plasma pretreatment and cocatalyst may have compensated for the reduction in the mechanical strength caused by the wrinkle-resistance agents. In this article, the optimum conditions for the plasma pretreatment on the basis of the result of the wrinkle-recovery angle were analyzed with an L 9 (3) 3 orthogonal array testing strategy technique. The results showed that plasma treatment conditions with (1) a 10 mm/s speed, (2) a 0.1 L/min oxygen flow rate, and (3) a 4-mm jet-to-substrate distance together caused a significant improvement in the wrinkle-resistance properties of the cotton fibers treated with the three different BTCA treatments. Moreover, the treatment speed was the dominant factor, followed by jet-to-substrate distance and oxygen flow rate, in affecting the extent of improvement.