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We report a new approach for the synthesis of multifunctional Au core@Prussian Blue analogous (PBA) shell nanoheterostructures that involves PBA shell growth on the surface of cyanide-stabilized gold nanoparticles. It permits the assembly of Au@KNiII[FeII(CN)6] core@shell and Au@KNiII[FeII(CN)6]@KNiII[CrIII(CN)6] core@shell@shell heterostructures with well-defined and size-controlled gold cores and PBA shells. These heterostructures exhibit tunable size- and shape-dependent magnetic and optical properties: (i) the surface plasmon resonance band position and intensity mainly depend on the PBA shell thickness, and (ii) the magnetic properties (the transition temperature, the coercivity, and magnetic regime) depend in a complex manner on the thickness as well as the particular morphology of the magnetic shell. [ABSTRACT FROM AUTHOR]

The rational design of well‐defined core–shell gold Prussian‐blue analogous nanoparticles is presented together with an in‐depth study of their optical and magnetic properties. It is shown that both properties may be tuned by modifying various parameters. This approach constitutes a first step towards the design of Prussian‐blue analogous magnetoplasmonic heterostructures. The cover artwork was designed by Mr. S. Bertrand. More information can be found in the Full Paper by J. Long and J. Larionova et al. on page 7483. [ABSTRACT FROM AUTHOR]