The valley degree of freedom in many-valley semiconductors provides a new paradigm for storing and processing information in valleytronic and quantum-computing applications. Achieving practical devices requires all-electric control of long-lived valley-polarized states, without the use of strong external magnetic fields. Because of the extreme strength of the carbon–carbon bond, diamond possesses exceptionally stable valley states that provide a useful platform for valleytronic devices. Using ultrapure single-crystalline diamond, we demonstrate electrostatic control of valley currents in a dual-gate field-effect transistor, where the electrons are generated with a short ultraviolet pulse. The charge current and the valley current measured at the receiving electrodes are controlled separately by varying the gate voltages. We propose a model to interpret experimental data, based on drift-diffusion equations coupled through rate terms, with the rates computed by microscopic Monte Carlo simulations. As an application, we demonstrate valley-current charge-state modulation of nitrogen-vacancy centers.