This study examines the predictive capability of our recently proposed reaction mechanism (Norinaga and Deutschmann, Ind Eng Chem Res 2007, 46, 3547) for hydrocarbon pyrolysis at varying temperature. The conventional flow reactor experiments were conducted at 8 kPa, over the temperature range 1073-1373 K, using ethylene, acetylene, and propylene as reactants to validate the mechanism. More than 40 compounds were identified and quantitatively analyzed by on- and off-line gas chromatography. The chemical reaction schemes consisting of 227 species and 827 reactions were coupled with a plug-flow reactor model that incorporated the experimentally measured axial temperature profile of the reactor. Comparisons between the computations and the experiments are presented for more than 30 products including hydrogen and hydrocarbons ranging from methane to coronene as a function of temperature. The model can predict the compositions of major products (mole fractions larger than 10-2) in the pyrolysis of three hydrocarbons with satisfactory accuracies over the whole temperature range considered. Mole fraction profiles of minor compounds including polycyclic aromatic hydrocarbons (PAHs) up to three ring systems, such as phenanthrene, anthracene, and phenylnaphthalene, are also fairly modeled. At temperatures lower than 1273 K, larger PAHs were underpredicted and the deviation became larger with decreasing temperature and increasing molecular mass of PAHs, while better agreements were found at temperatures higher than 1323 K. © 2008 Wiley Periodicals Inc.