AbstractFast neutron and X‐ray imaging are considered complementary nondestructive detection technologies. However, due to their opposite cross‐sections, development of a scintillator that is sensitive to both fast neutrons and X‐rays within a single‐material framework remains challenging. Herein, an organic–inorganic hybrid perovskite (C4H9NH3)2PbBr4 (BPB) is demonstrated as a scintillator that fully meets the requirements for both fast neutron and X‐ray detection. The hydrogen‐rich organic component acts as a fast neutron converter and produces detectable recoil protons. The heavy atom‐rich inorganic fraction efficiently deposits the energy of charged recoil protons and directly provides a large X‐ray cross‐section. Due to the synergy of these organic and inorganic components, the BPB scintillator exhibits high light yields (86% of the brightness of a commercial ZnS (Ag)/6LiF scintillator for fast neutrons; 22 000 photons per MeV for X‐rays) and fast response times (τdecay = 10.3 ns). More importantly, energy‐selective fast neutron and X‐ray imaging are also demonstrated, with high resolutions of ≈1 lp mm−1 for fast neutrons and 17.3 lp mm−1 for X‐rays; these are among the highest resolution levels for 2D perovskite scintillators. This study highlights the potential of 2D perovskite materials for use in combined fast neutron and X‐ray imaging applications.
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