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A GaN-based pin neutron detector with a 6LiF conversion layer was fabricated, and can be used to detect thermal neutrons. Measurement of the electrical characteristic of the GaN-based pin neutron detector showed that the reverse leakage current of the neutron detector was reduced significantly after deposition of a 6LiF conversion layer on the detector surface. The thermal neutrons used in this experiment were obtained from an 241Am–Be fast neutron source after being moderated by 100-mm-thick high-density polyethylene. The experimental results show that the detector with 16.9-μm thick 6LiF achieved a maximum neutron detection efficiency of 1.9% at a reverse bias of 0 V, which is less than the theoretical detection efficiency of 4.1% calculated for our GaN neutron detectors.