Nuclear magnetic resonance measurements of the 45 Sc, 1 H, and 2 D spin-lattice relaxation rates in the solid solutions ␣-ScH x (xϭ0, 0.11, and 0.27͒ and ␣-ScD x (xϭ0.05 and 0.22͒ have been performed over the temperature range 4.2-294 K. For the hydrided and deuterided samples we have found pronounced deviations of the 45 Sc relaxation rate measured at 86.2 MHz from the Korringa behavior in the range 30-180 K. The excess 45 Sc relaxation rate displays a peak near 100 K in ␣-ScH x and near 110-140 K in ␣-ScD x , resulting from the quadrupole interaction modulated by fast localized hopping of H͑D͒ atoms. The amplitude of the 45 Sc relaxation rate peak in the deuterided samples is found to be much higher than in the hydrided samples with comparable hydrogen content. This unusual isotope effect indicates that the fraction of D atoms participating in the fast localized motion in ␣-ScD x is approximately six times as large as the corresponding fraction of H atoms in ␣-ScH x . The results of our measurements of the 1 H and 2 D relaxation rates are consistent with this conclusion. The strong effect of H↔D substitution on the fraction of atoms involved in the localized hopping should be accounted for in any microscopic model of hydrogen motion in Sc. ͓S0163-1829͑99͒15725-4͔