A combined catalyst and sorbent was prepared and utilized for steam reforming methane and propane in laboratory-scale systems. The material was prepared in the form of small spherical pellets having a layered structure such that each pellet consisted of a highly reactive lime or dolime core enclosed within a porous but strong protective shell made of alumina in which a nickel catalyst was loaded. The material served two functions by catalyzing the reaction of hydrocarbons with steam to produce hydrogen while simultaneously absorbing carbon dioxide formed by the reaction. The in situ removal of CO 2 shifted the reaction equilibrium toward increased H 2 concentration and production. The concept was proved by using both a thermogravimetric analyzer and a fixed-bed reactor loaded with the material to reform hydrocarbons. Tests conducted with the fixed-bed reactor at atmospheric pressure and with temperatures in the range of 520-650°C produced a product containing a large concentration of H 2 (e.g., 94-96 mol %) and small concentration of CO and CO 2. Therefore, the results achieved in a single step were as good as or better than those achieved in a conventional multistep reaction and separation process.