C4 alkenes are generally used to produce synthetic rubbers, plastics, and other important chemicals. Transition metal oxides are traditionally used as catalysts to produce C4 alkenes from n-butane by oxidative dehydrogenation (ODH). On the other hand, metal-free carbon nanomaterials are receiving much attention as catalysts for ODH due to their environmental benignity, corrosion resistance, and unique surface properties. In this work, a systematic methodology was designed to measure conversion of the reactants, selectivity to main products, and other catalytic performances of a set of carbon catalysts, including graphite and activated carbon. The experiments were carried out under a wide range of reaction conditions, and the reaction mechanism and kinetics were developed based on Marsvan Krevelen interpretation of the experimental results.