Atmospheric nitrogen (N) and sulfur (S) deposition in subtropical forests has increased rapidly and the current level is very high, thus seriously affecting nutrient (e.g., N and phosphorus (P)) release from litter. However, the specific effects of S addition and its interaction with N on the release of carbon (C), N, and P from litter in subtropical evergreen broadleaved forests are unclear. Therefore, a two-year field experiment was performed using a litterbag method in a subtropical evergreen broadleaved forest in western China to examine the responses of litter decomposition and nutrient release to the control (CK), added N (+N), added S (+S), and added N and S (+NS) treatments. The results showed that the remaining litter mass, lignin, cellulose, C, N, P, and litter N/P ratio were higher, whereas the litter C/N ratio and soil pH were lower in the fertilization treatments than in CK. The annual decomposition coefficients (k-values) in the +N, +S, and +NS treatments were 0.384 ± 0.002, 0.378 ± 0.002, and 0.374 ± 0.001 year−1, respectively, which were significantly lower than the k-values in CK (0.452 ± 0.005 year−1, p < 0.05). The remaining mass, lignin, cellulose, C, and litter N/P ratio were higher, whereas the soil pH was lower in the +NS treatment than in the +N and +S. The interactive effects of N addition and S addition on the remaining litter lignin, cellulose, C, N, and P; the litter C/N, C/P, and N/P ratios; and the soil pH were significant (p < 0.05). In conclusion, the addition of N and S synergistically decreased the degradation of lignin and cellulose and the release of C and N and increased the litter N/P ratio, suggesting that external N and S inputs synergistically slowed the release of C and N from litter and exacerbated litter P limitation during decomposition in this forest.