Sm0.5Ba0.5MnO3-δ (SBMO) has been synthesized with the Pechini method and investigated as an anode material of solid oxide fuel cells with H2 and methanol as fuels. A cubic perovskite structure is formed after reduction. The reduction process of SBMO is studied with X-ray photoelectron spectroscopy and temperature programmed reduction techniques. The electrical conductivities of an SBMO sample sintered at 950°C are 1.15 and 0.10Scm−1 at 850°C in air and H2, respectively. A single cell with an SBMO anode layer and a 300-μm La0.8Sr0.2Ga0.8Mg0.2O3-δ electrolyte layer exhibits a maximum power density (Pmax) of about 150mWcm−2 at 850°C with H2 as fuel. The electrical conductivity of the anode layer with methanol as fuel is improved by the moderate carbon deposition, and the Pmax increases to about 415mWcm−2. The cell fed with methanol also shows a promising stability.