We have pioneered the use of liquid polar organic molecules as alternatives to rigid gate-dielectrics for the fabrication of graphene field-effect transistors. The unique high net dipole moment of various polar organic molecules allows for easy manipulation of graphene’s conductivity due to the formation of an electrical double layer with a high-capacitance at the liquid and graphene interface. Here, we compare the performances of dimethyl sulfoxide (DMSO), acetonitrile, propionamide, and valeramide as polar organic liquid dielectrics in graphene field-effect transistors (GFETs). We demonstrate improved performance for a GFET with a liquid dielectric comprised of DMSO with high electron and hole mobilities of 154.0 cm2/Vs and 154.6 cm2/Vs, respectively, and a Dirac voltage <5 V.