The formation of Au-Pt bimetallic nanoparticles (NPs) through the pulsed laser-induced dewetting (PLiD) of Au-Pt bilayer thin films on patterned dimpled Ta substrates was reported. It has been found that the total bilayer film thickness plays a determining role in the size of the NPs, whereas the NP size does not change much with the different sputtering order and laser fluence. The dimple coverage, characterizing the formation of NP arrays, depends mainly on the comparison of the NP diameter to the dimple size. Better overall coverages up to >90% were achieved from the NPs produced from PLiD of the two thinner films, i.e., Au(1.5 nm)Pt(1.5 nm) and Pt(1.5 nm)Au(1.6 nm). The energydispersive X-ray (EDX) spectroscopic analysis confirmed the presence of bimetallic Au-Pt NPs after dewetting. The X-ray photoelectron spectroscopic (XPS) measurements and electrochemical characterization using cyclic voltammetry of the produced bimetallic Au-Pt NPs both showed increased Au surface contents after PLiD, providing strong evidence for the formation of Pt-rich core/Au-rich shell NPs. The investigation of the electrochemical properties revealed stronger Pt−O bonding on the bimetallic Au-Pt NP surfaces. Furthermore, while Au is enriched on the Pt-rich core/Au-rich shell NP surfaces, a significant Pt content, ranging from 10% to close to 40%, is still present on the surface of the produced NPs, which could be useful for bifunctional electrocatalytic reactions.