Controlling the surface composition of shaped bimetallic nanoparticles could offer precise tunability of geometric and electronic surface structure for new nanocatalysts. To achieve this goal, a platform for studying the intermixing process in a shaped nanoparticle was designed, using multilayered Pd‐Ni‐Pt core–shell nanocubes as precursors. Under mild conditions, the intermixing between Ni and Pt could be tuned by changing layer thickness and number, triggering intermixing while preserving nanoparticle shape. Intermixing of the two metals is monitored using transmission electron microscopy. The surface structure evolution is characterized using electrochemical methanol oxidation. DFT calculations suggest that the low‐temperature mixing is enhanced by shorter diffusion lengths and strain introduced by the layered structure. The platform and insights presented are an advance toward the realization of shape‐controlled multimetallic nanoparticles tailored to each potential application.This is the peer-reviewed version of the following article: Williams, Benjamin P., Allison P. Young, Ilektra Andoni, Yong Han, Wei‐Shang Lo, Matthew Golden, Jane Yang, Lian‐Ming Lyu, Chun-Hong Kuo, James W. Evans, Wenyu Huang, and Chia-Kuang Tsung. "Strain‐Enhanced Metallic Intermixing in Shape‐Controlled Multilayered Core–Shell Nanostructures: Toward Shaped Intermetallics." Angewandte Chemie International Edition 59, no. 26 (2020): 10574-10580, which has been published in final form at DOI: 10.1002/anie.202001067. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving. Posted with permission.</p
