Energetic charged particles, such as galactic cosmic rays (GCRs) and solar energetic particles (SEPs), can penetrate deep within the lunar surface, resulting in deep dielectric charging. This charging process depends on the GCR and SEP currents, as well as on the regolith's electrical conductivity and permittivity. In permanently shadowed regions (PSRs) near the lunar poles, the discharging timescales are on the order of a lunation (∼20 days). We present the first predictions for deep dielectric charging of lunar regolith. To estimate the resulting subsurface electric fields, we develop a data‐driven, one‐dimensional, time‐dependent model. For model inputs, we use GCR data from the Cosmic Ray Telescope for the Effects of Radiation on board the Lunar Reconnaissance Orbiter and SEP data from the Electron, Proton, and Alpha Monitor on the Advanced Composition Explorer. We find that during the recent solar minimum, GCRs create persistent electric fields up to ∼700 V/m. We also find that large SEP events create transient but strong electric fields (≥106 V/m) that may induce dielectric breakdown. Such breakdown would likely result in significant modifications to the physical and chemical properties of the lunar regolith within PSRs.