Metallic iron as a catalyst for tar cracking in biomass gasification has been investigated. Based on previous studies showing that iron must be in its elemental form to catalyze the tar breakdown reactions, thermodynamic calculations suggest the existence of an operating window where iron is neither oxidized nor contaminated by carbon deposits. A straightforward biomass gasification model has been derived and used in conjunction with thermodynamics for making plots that illustrate the mentioned operating window, which is achievable under real conditions. Experiments made under these specific calculated conditions confirm that elemental iron effectively acts as a tar breakdown catalyst, resulting in an improved gas yield and a decrease in tar concentration. The desired operating window is governed mainly by adjusting the oxygen input (i.e., the equivalence ratio) and the temperature.