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We report the controllable synthesis of AuNi core-shell (c-AuNi) and Janus (j-AuNi) nanocrystals (NCs) with uniform shape, tunable size and compositions in the presence of trioctylphosphine (TOP) or triphenylphosphine (TPP). The morphology of the AuNi bimetallic NCs could be regulated by varying the structure and concentration of phosphine ligands. The ligand-directed structural evolution mechanism of AuNi bimetallic NCs was investigated and discussed in detail.

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