The negative capacitance frequently observed at low frequencies in organic light-emitting diodes (LEDs) is explained as a signature of sequential electron injection at the organic/metal interface first to states in the bandgap in the dipole layer and then to bulk states. The negative capacitance occurs when the interfacial states depart from equilibrium with the metal Fermi level due to an increasing rate of hopping to the bulk states. A simple kinetic model compares well with the experimental results and provides a new tool to investigate interfacial properties for improving the performance of organic LEDs. (c) 2006 Elsevier B.V. All rights reserved.