By pretreating the substrate of a graphene field-effect transistor (G-FET), a stable unipolar transfer characteristic, instead of the typical V-shape ambipolar behavior, has been demonstrated. This behavior is achieved through functionalization of the SiO 2 /Si substrate that changes the SiO 2 surface from hydrophilic to hydrophobic, in combination with postdeposition of an Al 2 O 3 film by atomic layer deposition (ALD). Consequently, the back-gated G-FET is found to have increased apparent hole mobility and suppressed apparent electron mobility. Furthermore, with addition of a top-gate electrode, the G-FET is in a double-gate configuration with independent top-or backgate control. The observed difference in mobility is shown to also be dependent on the top-gate bias, with more pronounced effect at higher electric field. Thus, the combination of top and bottom gates allows control of the G-FET's electron and hole mobilities, i.e., of the transfer behavior. Based on these observations, it is proposed that polar ligands are introduced during the ALD step and, depending on their polarization, result in an apparent increase of the effective hole mobility and an apparent suppressed effective electron mobility.