In this study, Eu:6LiBr/BaBr2 with a high Li concentration was developed as a novel neutron scintillator. Here, an Eu-doped BaBr2 phase acted as a scintillator and 6Li-containing LiBr phase acted as a neutron capturer. Eu:6LiBr/BaBr2 eutectics were fabricated via the vertical Bridgman technique in quartz ampoules. The scintillation performance of Ce:6LiBr/LaBr3 was measured using electron and neutron irradiation to evaluate its potential as a neutron scintillator. The grown Eu:6LiBr/BaBr2 eutectic exhibited a lamellar eutectic structure and optical transparency as well as a 410 nm emission due to the Eu2+ 5d–4f transition. The light yield under thermal neutron excitation was estimated to be 5600 photons/neutrons. The scintillation decay time was 550 ns.