State-of-the-art thermal neutron scintillation detectors rely on rare isotopes for neutron capture, lack stability and scalability of solid-state scintillation devices, and poorly discriminate between the neutron and gamma rays. The boron nitride (BN)-CsPbBr 3 perovskite nanocomposite aerogel scintillator enables discriminative detection of thermal neutrons, features the largest known size (9 cm across), the lowest density (0.17 g cm −3 ) among the existing scintillation materials, high BN (50%) perovskite (1%) contents, high optical transparency (85%), and excellent radiation stability. The new detection mechanism relies on thermal neutron capture by 10 B and effective energy transfer from the charged particles to visible-range scintillation photons between the densely packed BN and CsPbBr 3 nanocrystals. Low density minimizes the gamma ray response. The neutrons and gamma rays are discriminated by complete decoupling of the respective single pulses in time and intensity. These outcomes open new avenues for neutron detection in resource exploration, clean energy, environmental, aerospace, and homeland security applications.