Engineering nanomaterials at single-atomic sites could enable unprecedented catalytic properties for broad applications, yet it remains challenging to do so on the surface of multimetallic nanocrystals. Herein, we present the multifactorial engineering (size, shape, phase, and composition) of the fully ordered PtBi nanoplates at atomic level, achieving a unique catalyst surface where the face-centered cubic (fcc) Pt edges are modified by the isolated Pd atoms and BiO