Previous first-principles calculations have failed to reproduce many of the key thermoelectric features of Fe 2 VAl, e.g. the maximum values of the Seebeck coefficient S and its asymmetry with respect to the chemical potential. Also, previous theoretical predictions suggested that the pseudo band gap of Fe 2 VAl switches from indirect to direct upon doping. In this work, we report first-principles calculations that correctly reproduce the experimentally measured thermoelectric properties of Fe 2 VAl. This is achieved by adding a larger Hubbard U term to V atoms than to Fe atoms and including a scissors operator afterwards. As a result, bulk Fe 2 VAl is modelled as a gapless semiconductor with maximum S values of 76 and −158 µV/K for p-and n-type, respectively, which agree well with the experimental measurements.