Pt monolayers (Pt ML ) supported on nanoparticles with different compositions (i.e., Ru, Rh, Pd, Ir, and Au) were synthesized by the surface-limited redox replacement of underpotentially deposited Cu monolayers on nanoparticle supports. Nanoparticle supports with different compositions were directly deposited on the conducting substrate by a clean and one-step electrodeposition method with controlled deposition potential and time. The whole synthesis process of the electrode was free of surfactants, binders, capping agents and reductants, and without an additional coating process of electrocatalysts. The results show that the specific activity (SA) of Pt ML electrocatalysts depended strongly on the composition of the nanoparticle support. For example, the Pt ML supported on the Au nanoparticle exhibited 8.3 times higher SA than that supported on the Ru and Pd nanoparticles. The change in the SA of the Pt ML supported on different nanoparticles was related to the substrate-induced strain in the Pt ML resulting from the lattice mismatch between the Pt ML and the nanoparticle support. As the strain in the Pt ML changed from the tensile strain to the compressive strain, the SA of the Pt ML electrocatalysts decreased remarkably.