We report attaining Ga‐terminated (4×2) surface reconstruction on virgin GaAs substrates using a completely dry process at temperatures below the oxide sublimation temperature and without group V overpressure. The native oxides are removed with an electron cyclotron resonance hydrogen plasma treatment, followed by annealing at 500 °C in ultrahigh vacuum, which yields a reconstructed surface suitable for epitaxial overgrowth. Characterization by secondary ion mass spectroscopy and transmission electron microscopy reveals the complete removal of O, reduced C, and high structural order at the epilayer/substrate interface when this preparation method is used before molecular beam epitaxy. Annealing the substrate at a lower temperature yields a nonreconstructed surface possessing significant impurity concentrations, and leads to dislocation defects at the epilayer/substrate interface.