In this paper, we report 591 high-velocity star candidates (HiVelSCs) selected from over 10 million spectra of Data Release 7 (DR7) of the Large Sky Area Multi-object Fiber Spectroscopic Telescope and the second Gaia data release, with three-dimensional velocities in the Galactic rest frame larger than 445 km s?1. We show that at least 43 HiVelSCs are unbound to the Galaxy with escape probabilities larger than 50%, and this number decreases to eight if the possible parallax zero-point error is corrected. Most of these HiVelSCs are metal-poor and slightly α-enhanced inner halo stars. Only 14% of them have [Fe/H]?>??1, which may be the metal-rich “in situ” stars in the halo formed in the initial collapse of the Milky Way or metal-rich stars formed in the disk or bulge but kinematically heated. The low ratio of 14% implies that the bulk of the stellar halo was formed from the accretion and tidal disruption of satellite galaxies. In addition, HiVelSCs on retrograde orbits have slightly lower metallicities on average compared with those on prograde orbits; meanwhile, metal-poor HiVelSCs with [Fe/H]?