We report on a new technique, spin-polarized electron emission spectroscopy. Using grazing-angle, surface scattering of H+ and He+ ions at Ni(110), we find that the angle-resolved energy distribution of emitted spin-polarized electrons is significantly different from that of electron-induced secondary (cascade) electrons and exhibits a series of characteristic ‘‘peaks’’ (including element-specific Auger electrons). We obtain characteristic, spin-dependent information on the surface electronic structure of Ni(110) and on atom-surface charge-transfer processes.