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In this Letter, a rational and stepwise method for the solution-phase synthesis of asymmetric Au split nanorings by adopting Au nanoprisms as a template has been demonstrated. The selective chemical etching of Au nanoprism tips activated the surface reactivity of edges and led to the selective deposition of Pt at the periphery of Au nanoplates. By controlling the total amount of Pt on the edges, different degrees of split Au@Pt nanorings were obtained; the subsequent Au coating around the Au@Pt scaffold eventually resulted in asymmetric Au hexagonal split nanorings. Their surface plasmonic features as a function of split degrees were investigated, including straight nanorods, bent nanorods, split nanorings, and full nanorings. The electrical field focusing using single-particle surface-enhanced Raman spectroscopy was evaluated under different polarization angles of the incident light for two different structures with the point gap and line gap between two arms.