In this work, Pb 3 B 10 O 16 [OH] 4 single crystal nanosheets are fabricated by a solvothermal process. Its structure is determined in detail by XRD, SEM, and TEM. The nanosheets display a good ability to attenuate both neutron and gamma radiations. In particular, it provides a distinct advantage to attenuate the gamma radiation with low energy from 59 to 105 keV. Notably, the lead borate single crystals with 2D nanostructures impliy other benefits, such as mechanical enhancement and high thermal conductivity. Thus, the lead borate nanosheets can be applied to the fabrication of multifunctional integrated composites for the radiation protection of complex conditions.