Controlling the crystal structure of GaN as either cubic (c-) or hexagonal (h-) GaN by changing the electric bias during growth was studied. After growth, we used transmission electron microscopy (TEM) and X-ray diffraction to determine the microstructure of c-GaN and h-GaN. Although c-GaN was confirmed, the interface at h-GaN/c-GaN was not clear. To increase the transition rates of crystal structure at the interface, we added hydrogen as a hydrogen-nitrogen mixed gas plasma while changing the electric bias. When we introduced hydrogen for 20 s while simultaneously changing the electric bias from 20 to 0 V, the crystal structure of GaN changed abruptly from cubic to hexagonal. TEM observations showed that the interface contained a thin layer with a high density of stacking faults, indicating that addition of hydrogen clearly assisted the change of crystal structure by forming stacking faults.Introduction GaN is well known to crystallize in two types of crystal structures. One is the hexagonal wurtzite structure with ABABAB stacking sequence and the other is the cubic zincblende structure with ABCABC stacking. At high growth temperatures, such as about 1000 C for metal organic chemical vapor deposition (MOCVD), GaN generally crystallizes in the hexagonal structure. Thus, recent light emitting diodes and laser diodes fabricated by MOCVD are based on hexagonal GaN (h-GaN) [1]. However, for fabrication of laser diodes with cleaved mirrors, cubic GaN (c-GaN) has an advantage over h-GaN. In addition, c-GaN is expected to have better electrical properties [2] resulting from its smaller effective masses and reduced phonon scattering in its higher crystallographic symmetry. With these advantages as a background, a large number of studies to obtain high-quality c-GaN have been carried out [3]. Yang et al. [4] attempted an intriguing sequential growth method for h-GaN and c-GaN on GaAs (111) substrates by varying the substrate temperature during growth. In our previous study, cGaN was obtained by changing the electric bias voltages applied to the sapphire (0001) substrates during GaN growth by electron-cyclotron-resonance plasma-excited molecular beam epitaxy (ECR-MBE) [5,6]. The bias voltage-mediated method should have an advantage over the temperature-mediated method because the former is much quicker and simpler than the latter; hence, the bias voltage method has the potential to grow sharp hexagonal and cubic interfaces and superlattice structures. In this paper, we report on the growth of multilayer structures of c-GaN and h-GaN that were made by changing the electric bias during growth. The c-GaN and h-GaN were characterized using transmission electron microscopy (TEM) and X-ray diffraction (XRD). Effects from adding hydrogen during the electric bias change are also discussed.