A single crystal of YAl3(BO3)4 was grown using the top-seeded solution growth method. The vacuum ultraviolet (VUV) excitation spectrum, monitored at the emission wavelength of 312 and 372 nm, showed a narrow excitation band at around 162 nm, which is located near the absorption edge of the YAl3(BO3)4 host. Upon VUV excitation at 162 nm, the characteristic self-trapped exciton (STE) emission bands were observed at 312 and 372 nm. The X-ray excited scintillation spectrum shows a broad emission band peaking at 310 nm with a weak shoulder band at around 375 nm, which is consistent with photoluminescence, and can thus be assigned to the STE emission. The scintillation light yield under irradiation at a 252Cf-thermal neutron reached 2700 photons/thermal neutron.