<jats:title>Abstract</jats:title><jats:p>It is widely recognized that the effect of doping into a Mott insulator is complicated and unpredictable, as can be seen by examining the Hall coefficient in high <jats:italic>T</jats:italic><jats:sub>c</jats:sub> cuprates. The doping effect, including the electron–hole doping asymmetry, may be more straightforward in doped organic Mott insulators owing to their simple electronic structures. Here we investigate the doping asymmetry of an organic Mott insulator by carrying out electric-double-layer transistor measurements and using cluster perturbation theory. The calculations predict that strongly anisotropic suppression of the spectral weight results in the Fermi arc state under hole doping, while a relatively uniform spectral weight results in the emergence of a non-interacting-like Fermi surface (FS) in the electron-doped state. In accordance with the calculations, the experimentally observed Hall coefficients and resistivity anisotropy correspond to the pocket formed by the Fermi arcs under hole doping and to the non-interacting FS under electron doping.</jats:p>
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