As graphene field-effect transistors (GFETs) are becoming increasingly valued for sensor applications, efficiency and control of their surface functionalization become critical. Here, we introduce an innovative method using a gate electrode to precisely modulate aryldiazonium functionalization directly on graphene devices. Although this covalent chemistry is well-known, we show that its spontaneous reaction on GFETs is highly heterogeneous with a low overall yield. By dynamically tuning the gate voltage in the presence of the reactant, we can quickly enable or suppress the reaction, resulting in a high degree of homogeneity between devices. We are also able to monitor and control functionalization kinetics in real time. The mechanism for our approach is based on electron transfer availability, analogous to chemical, substrate-based, or electrochemical doping, but has the practical advantage of being fully implementable on devices or chips. This work illustrates how powerful the FET platforms are to study surface reactions on nanomaterials in real time.