This study investigates the broad-energy-spectrum reactor-neutron irradiation effects on the electrical characteristics of Ni/β-Ga2O3 Schottky barrier diodes (SBDs), where the irradiated neutron fluence was up to 1 × 1016 cm−2. On the one hand, the high neutron fluence of 1016 cm−2 resulted in a reduction in forward current density by two orders of magnitude and an extremely high on-resistance property due to the radiation-generated considerable series resistance in the SBD. On the other hand, the irradiation brought little influence on the Ni/β-Ga2O3 Schottky contact, since the extracted ideality factor and barrier height from temperature-dependent current–voltage (I–V–T) characteristics showed no significant changes after the radiation. Moreover, the capacitance–voltage (C–V) characterization revealed that the net carrier density in the β-Ga2O3 material was only reduced by 25% at the neutron fluence of 1015 cm−2 but a significant reduction by 2–3 orders at 1016 cm−2. Within the neutron fluence range of 2 × 1014 cm−2 up to 1016 cm−2, the carrier removal rates trended to be saturated with the increased fluences, following an exponential regular. In addition, the C–V measurement on the 1016 cm−2 irradiated sample exhibited an obvious frequency dispersion, and the extracted carrier distribution was not uniform.