Studies exploring how vibrational energy (E-vib) promotes chemical reactivity most often focus on molecular reagents, leaving the role of substrate atom motion in heterogeneous interfacial chemistry underexplored. This combined theoretical and experimental study of methane dissociation on Ni(111) shows that lattice atom motion modulates the reaction barrier height during each surface atoms vibrational period, which leads to a strong variation in the reaction probability (S-0) with surface temperature (T-surf). State-resolved beam-surface scattering studies at T-surf = 90 K show a sharp threshold in S-0 at translational energy (E-trans) = 42 kJ/mol. When Etrans decreases from 42 kJ/mol to 34 kJ/mol, S-0 decreases 1000-fold at T-surf = 90 K, but only 2-fold at T-surf = 475 K. Results highlight the mechanism for this effect, provide benchmarks for DFT calculations, and suggest the potential importance of surface atom induced barrier height modulation in heterogeneously catalyzed reactions, particularly on structurally labile nanoscale particles and defect sites.