<p>Gallium is widely used now in different modern technological applications. Here we report studies of orientational crystallization of gallium in strong magnetic field. We used a Bruker Avance 400 NMR spectrometer to reveal the growth of the single crystalline α-Ga upon freezing the melt in magnetic field of the spectrometer. The particular orientations of the crystalline axes for solid gallium were evidenced in situ by the appearance of narrow resonance lines, specific for single crystals, and by the angular dependences of the NMR lineshifts. The resonance lines corresponded to the central and satellite transitions were observed. Measurements were carried out for both gallium isotopes, ⁷¹Ga and ⁶⁹Ga. The NMR results were confirmed by X-ray diffraction. A set of 23 gallium samples were studied. All samples demonstrated the formation of single crystalline structures with the (100), (113), (111), and (104) planes aligned perpendicular to the magnetic field. The narrow satellite lines proved the high quality of the crystals.</p>