Here we describe a strategy to fabricate multifunctional graphene-polymer hybrid thin-film transistors (PG-TFT) whose transport properties are tunable by varying the deposition conditions of liquid-phase exfoliated graphene (LPE-G) dispersions onto a dielectric surface and via thermal annealing post-treatments. In particular, the ionization energy (IE) of the LPE-G drop-cast on SiO2 can be finely adjusted prior to polymer deposition via thermal annealing in air environment, exhibiting values gradually changing from 4.8 eV up to 5.7 eV. Such a tunable graphene’s IE determines dramatically different electronic interactions between the LPE-G and the semiconducting polymer (p- or n-type) sitting on its top, leading to devices where the output current of the PG-TFT can be operated from being completely turned off up to modulable. In fact upon increasing the surface coverage of graphene nanoflakes on the SiO2 the …