In this research, core-shell electrocatalysts comprising a Ru core covered with precisely controlled 1.5-3.6 atomic layers (ALs)-thick Pt atoms are synthesized. The sample with 1.5 ALs shows a 3.2-fold improvement in CO-tolerance and 2.4-fold current enhancement at the conventional battery operation potential (I(300), at 300 mV vs Ag/AgCl) during methanol oxidation as compared with conventional all-Pt nanoparticles. The origin of the enhanced performance and the atomic structure of the core-shell nanoparticles are elucidated to be mainly dominated by the lattice strain (possibly some slight effect of heteroatomic interactions) then by the combination of ligand effects and bifunctional mechanisms when the shell crystal is thicker than 2.7 ALs.