We investigated the property of GaN crystals under a strong electric field. The Raman spectra of GaN were measured using an ultraviolet laser, and a remarkable redshift of the A 1 (LO) mode was observed. The role of the surface depletion layer was discussed, and the interrelation between the electric field and phonons was revealed. First-principles calculations indicated that, in particular, the phonons that vibrate along the [0001] direction are strongly influenced by the electric field. This effect was confirmed by a surface photovoltage experiment. The results revealed the origin of the redshift and presented the phonon property of GaN under a strong electric field.