The neutral fractions were measured for 50–250 keV hydrogen emerging from a NiSi2(111) surface at several grazing exit angles (the angle between the outgoing hydrogen and the surface). It was found first that the neutral fractions depend strongly on the exit angle, and the values become close to that for pure Si as the energy and the exit angle of the emitting hydrogen decrease. We compared the experimental results with the ones calculated by assuming that NiSi2consists of dense atomic layers of Si and Ni. The best fit is obtained with the structural model in which the topmost layer is composed of Si atoms and the second one is Ni atoms.