Recently reported molecular ion/surface scattering experiments [J. Chem, Phys, 100, 6791 (1994)] demonstrate that the translational and vibrational energies of incident NO+ each have a distinct influence on molecular dissociation for the NO+/GaAs(110) system. The detailed analysis of possible mechanisms suggest that the initial translational, vibrational, and rotational energies, as well as the molecule’s orientation and point of impact at the surface are important in determining the dissociation probability. In this paper, a wave packet simulation of NO+/GaAs(110) scattering is performed. The emphasis in the study is on the branching ratio for production of NO, NO-, O, and O- as a function of vibrational and translational energy of the incident NO+. A novel procedure for treating the coupling of a molecular state with a band of substrate electronic states is combined with a mixed classical-quantal treatment of the nuclear motion. The simulations suggest that electron transfer and collision induced dissociation (CID) cooperate and form a vibrational coherence through which the initial vibrational state strongly influences the dissociation dynamics.