Electro-optic modulation at frequencies of 100 GHz and beyond is important for photonic-electronic signal processing at the highest speeds. To date, however, only a small number of devices exist that can operate up to this frequency. In this study, we demonstrate that this frequency range can be addressed by nanophotonic, silicon-based modulators. We exploit the ultrafast Pockels effect by using the silicon–organic hybrid (SOH) platform, which combines highly nonlinear organic molecules with silicon waveguides. Until now, the bandwidth of these devices was limited by the losses of the radiofrequency (RF) signal and the RC (resistor-capacitor) time constant of the silicon structure. The RF losses are overcome by using a device as short as 500 µm, and the RC time constant is decreased by using a highly conductive electron accumulation layer and an improved gate insulator. Using this method, we demonstrate for the first time an integrated silicon modulator with a 3dB bandwidth at an operating frequency beyond 100 GHz. Our results clearly indicate that the RC time constant is not a fundamental speed limitation of SOH devices at these fr ... mehrequencies. Our device has a voltage–length product of only VπL=11 V mm, which compares favorably with the best silicon-photonic modulators available today. Using cladding materials with stronger nonlinearities, the voltage–length product is expected to improve by more than an order of magnitude.