Monte Carlo simulations are reported to predict the dependence of the surface tension of water–alcohol mixtures on the alcohol concentration. Alcohols are modeled using the anisotropic united atom model recently extended to alcohol molecules. The molecular simulations show a good agreement between the experimental and calculated surface tensions for the water–methanol and water–propanol mixtures. This good agreement with experiments is also established through the comparison of the excess surface tensions. A molecular description of the mixture in terms of density profiles and hydrogen bond profiles is used to interpret the decrease of the surface tension with the alcohol concentration and alcohol chain length.