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Electrical and optical properties of GaAs layers are improved by applying substrate bias during electron‐cyclotron‐resonance plasma‐excited molecular beam epitaxy (ECR‐MBE). The highest mobility obtained without substrate bias is 4500 cm2 V-1 s-1. By applying positive bias, the mobility of the grown layer is increased to as high as 6800 cm2 V-1 s-1. Intense photoluminescence spectra comparable to that of a high quality MBE‐grown layer are also observed. The suppression of high‐energy ion impingement on the growing surface plays an important role in obtaining high quality crystal.