Lowering the oxygen content in biofuels is of vital importance, since high oxygen level content leads to low stability, low heat value, and corruption in engines. Here we report on the thermally activated decarboxylation of fatty acids, raw materials for biofuel production, on an anisotropic Au(110) surface. Due to the one-dimensional (1D) geometrical constraint of the surface reconstruction, linear fatty acid molecules (C 30 H 60 O 2 ) are decarboxylated and polymerized at their terminal ends at mild temperatures, resulting in the formation of oxygen-free aliphatic hydrocarbons. Different reaction stages of the decarboxylation were monitored by high-resolution scanning tunneling microscopy and X-ray photoemission spectroscopy. On the basis of density functional theory calculations, a two-step process was proposed for the fatty acid decarboxylation. Our work demonstrates a novel strategy for deoxygenation of fatty acids on a 1D constrained surface as a model catalytic system for producing low oxygen content biofuels.