We studied the adsorption and reaction of nitrogen dioxide gas on the surface of an ice film at temperatures of 100−170 K under ultrahigh vacuum (UHV) conditions. Cs + reactive ion scattering (RIS) and low-energy sputtering (LES) techniques were used to identify and quantify the reactants and products on the surface of the ice film, in conjunction with the use of temperature-programmed desorption (TPD) to monitor the species desorbed. Temperature-ramping experiments were performed to examine the changes in the populations of these species as a function of temperature. Adsorption of NO 2 gas on the ice film at <110 K produced physisorbed species that may possibly possess negative charge character (NO 2 δ-), as deduced from the NO 2 and NO 2 − signals in the RIS and LES experiments. At 110−130 K, NO 2 δ-species were either desorbed as NO 2 gas or converted to nitrous acid (HONO), NO 3 − , and H 3 O + on the surface. Nitrous acid gas was desorbed at 140−160 K. The efficiency of conversion of NO 2 to surface nitrous acid was about 40%, and that to nitrous acid gas was about 7%. The efficiency of the reaction of NO 2 on the ice surface may be higher than that at the gas/liquid water interface. The reaction efficiency increased with a decrease of the NO 2 coverage and was inversely correlated with the N 2 O 4 coverage, which favors the mechanistic interpretation that an isolated NO 2 molecule reacts with water. However, NO 2 can diffuse on the ice surface to form clusters at ≥120 K. Under these conditions, the possibility that dimerization of NO 2 contributes to the hydrolysis reaction of NO 2 may not be excluded.