The polymer materials in nuclear facilities are exposed to high temperatures, radiation, and high loads. Their excellent heat resistance, radiation resistance, and shielding properties are important for the safe operation of nuclear facilities. In this study, 1,2-bis(hydroxymethyl)carborane (CBOH) was first synthesized in large quantities through water extraction and then introduced into an epoxy resin cross-linked network. The incorporation of a carborane structure significantly improved the heat resistance of epoxy. Under air atmosphere, the T 5% (the temperature at 5 wt % degradation), T 10% (the temperature at 10 wt % degradation), and char yield at 800 °C of the materials were 315.67 °C (16.51 °C increased), 326.29 °C (12.96 °C increased), and 33.22% (33.22% increased), respectively. The maximum decomposition temperature of the material increased from 550 to 750 °C, and 7.05 wt % of the carbon constituent was protected after thermal degradation at 800 °C. The glass transition temperature (T g ) of the materials greatly increased up to over 300 °C after introducing the carborane structure into the networks. The radiation resistance of the material was enhanced due to the in situ capture of oxygen radicals by the carborane structure. Moreover, the incorporation of carborane structure also increased the content of H and B in materials, improving their neutron-shielding capability. This work confers multifunctionality to epoxy resin and enhances its various properties, ensuring the safety of epoxy resin in nuclear facilities.