On 17 March 2013, a large magnetic storm significantly depleted the multi-MeV radiation belt. We present multi-instrument observations from the Van Allen Probes spacecraft Radiation Belt Storm Probe A and Radiation Belt Storm Probe B at ~6 Re in the midnight sector magnetosphere and from ground-based ionospheric sensors during a substorm dipolarization followed by rapid reenergization of multi-MeV electrons. A 50% increase in magnetic field magnitude occurred simultaneously with dramatic increases in 100 keV electron fluxes and a 100 times increase in VLF wave intensity. The 100 keV electrons and intense VLF waves provide a seed population and energy source for subsequent radiation belt enhancements. Highly relativistic (>2 MeV) electron fluxes increased immediately at L* ~ 4.5 and 4.5 MeV flux increased >90 times at L* = 4 over 5 h. Although plasmasphere expansion brings the enhanced radiation belt multi-MeV fluxes inside the plasmasphere several hours postsubstorm, we localize their prompt reenergization during the event to regions outside the plasmasphere.