Here we report the growth of phase-pure InAs nanowires on Si (111) substrates by molecular-beam epitaxy using Ag catalysts. A conventional one-step catalyst annealing process is found to give rise to InAs nanowires with diameters ranging from 4.5 to 81 nm due to the varying sizes of the Ag droplets, which reveal strong diameter dependence of the crystal structure. In contrast, a novel two-step catalyst annealing procedure yields vertical growth of highly uniform InAs nanowires ∼10 nm in diameter. Significantly, these ultrathin nanowires exhibit a perfect wurtzite crystal structure, free of stacking faults and twin defects. Using these high-quality ultrathin InAs nanowires as the channel material of metal-oxide-semiconductor field-effect transistor, we have obtained a high I ON/I OFF ratio of ∼106, which shows great potential for application in future nanodevices with low power dissipation.