The concentrations of O, OH, and H//2O were measured during the reflected-shock initiated reaction of CH//4-O//2-Ar mixtures using various spectroscopic techniques. A proposed 23-reaction methane oxidation mechanism correctly predicts the time of occurrence and magnitude of the radical concentration overshoots, and also predicts a departure from a partial equilibrium state during the initial stages of the radical concentration overshoots. Rate constants for several elementary reactions in the proposed mechanism were inferred by a comparison of the observed and predicted concentration profiles.