Single crystals of Ce doped Li6Gd(BO3)3 (LGBO:Ce), Li6Lu(BO3)3 (LLBO:Ce), and Li6Y(BO3)3 (LYBO:Ce) are grown using the Czochralski technique. A comparison of the challenges faced in the growth of these materials in single crystalline form is discussed. The grown crystals are characterized for their thermal, structural, optical, and scintillation characteristics to explore their potential as thermal neutron detectors. Scintillator detectors based on LRBO:Ce (R = Gd, Lu, Y) crystals are used successfully to record the pulse‐height spectra from various gamma energies and thermal neutron sources in the flux range from 10 to 107 n (cm2 s)–1.