A self-dispersing pigment was produced by a diazonium coupling reaction; the pigment reacted with aromatic diazonium salts which were generated by the reaction of p-aminobenzene sulfonic acid and sodium nitrite. The surface of the pigment particles was negatively charged due to sulfonic acid groups on the pigment surface. The pigment particle size and zeta potential were, respectively, 134.5 nm and −45.4 mV at neutral pH. The wool surface was positively charged by adjusting the pH; then the anionic self-dispersing pigment dyed the cationic wool. The results show that self-dispersing pigment can adhere well without a binder, and that the K/S value is closely related to pH, dyeing time, and the amount of pigment. The color fastness of the wool was good and the light fastness of the wool was grade 5, which is better than acid dyes. Self-dispersing pigments are potential candidates for dyeing high-weather-resistance textiles.