We investigated electrolyte-gated graphene field-effect transistors (GFETs) for electrical detecting pH and protein adsorptions. Nonfunctionalized single-layer graphene was used as a channel. GFETs immersed in an electrolyte showed transconductances 30 times higher than those in a vacuum and their conductances exhibited a direct linear increase with electrolyte pH, indicating their potential for use in pH sensor applications. We also attempted to direct surface-protein adsorption and showed that the conductance of GFETs increased with exposure to a protein at several hundred picomolar. The GFETs thus acted as highly sensitive electrical sensors for detecting pH and biomolecule concentrations.