The surface structure, morphology, and crystallinity of high Miller index (511) and (711) GaAs epitaxial layers prepared by molecular‐beam epitaxy are studied with electron diffraction, scanning electron micorscopy, Raman scattering, and Rutherford backscattering. All A‐ and B‐(511) and (711) surfaces exhibit an ordered array of steps with (100) terraces and (111) risers. The (511)‐B layers exhibit the smoothest surface morphology, and the best surface and bulk crystallinity among these layers.