Although in principle semiconductor-metal (Schottky) diodes should be tunable by changing the work function of the metal, such flexibility cannot be achieved in a single device and in practice is often limited by interfacial states that cause Fermi-level pinning. A tunable diode is reported based on a hybrid inorganic-organic, n-indium phosphidepoly(pyrrole)nonaqueous electrolyte architecture. By electrochemically manipulating the work function of the conjugated polymer poly(pyrrole), the turn-on voltage (more precisely, the forward bias potential required to pass a particular current) of the diode can be continuously and actively tuned by more than 0.6 volt. The work highlights a distinguishing feature of conjugated polymers relative to more traditional semiconductor materials, namely, the ability of dopant ions to permeate conjugated polymers, thereby enabling electrochemical manipulation.