The reactions of CH and C-atoms with N2, which are believed to be initial steps in the prompt-NO mechanism, were studied at high temperature behind reflected shocks. CH was formed from the pyrolysis of highly dilute mixtures of CH4 or C2H6 (<30 ppm) in argon. C-atoms were formed by pyrolysis of dilute mixtures of C3O2 in argon. the reaction rates were determined from measurements of CH, C-atom and N-atom concentrations. CH was detected by cw, narrow-linewidth laser absorption of 431.131 nm. C-atoms and N-atoms were detected using atomic resonance absorption (ARAS) at 156.1 nm and 119.9 nm, respectively. Pyrolysis of C3O2 in the presence of excess N2 resulted in rapid C-atom removal due to C(3P)+N2→CN+N, (1) leading to k1=6.3×1013 exp(−23160 K/T) (±30%) cm3 mol−1 s−1 over the temperature range 2660 to 4660 K and pressure range 0.5 to 1 atm. In order to determine the rate coefficient of CH(X2II)+N2→HCN+N, (2) a perturbation technique was employed. In this technique, the CH profile resulting from pyrolysis of CH4 or C2H6 dilute in argon was perturbed by the addition of N2. A detailed analysis of the CH profiles led to a rate coefficient, k2=4.4×1012 exp(−11060 K/T)(±50%) cm3 mol−1 s−1 over the temperature range 2500 to 3800 K and pressure range 0.6 to 1 atm. N-atom measurements provided an independent verification of k2 and the products of reaction 2.