Nanoparticles can be used for decoration and functionalization of single polymer molecules that have been adsorbed to a solid substrate. Initial attempts to prepare Prussian Blue nanoclusters by a layer-by-layer deposition technique of hexacyanoferrate anions and ferric cations onto isolated polycation chains in water failed because of the desorption of the first layer upon deposition of the next one. A simple method for the preparation of charge-stabilized Prussian Blue nanoparticles of readily adjustable size is reported. Prussian Blue nanoparticles have been purified by addition of non-solvents and redispersed in water without aggregation. Thus formed Prussian Blue nanoparticles are crystalline and display a long-range ferromagnetic ordering at 5.1 K. Prussian Blue nanoparticles were selectively deposited along single polycation molecules to form a one-dimensional array or were attached to the surface of carbon nanotubes (CNTs) functionalized with poly2-vinylpyridine (P2VP). These nanoparticle-based nanostructures might be useful materials for manufacture of electrooptical devices, or mechanically robust ion-sieving membranes.