Physical and chemical properties of nanosized crystals are known to be a function of their size, morphology, and chemical composition. [1][2][3][4][5][6] Hence, over the past decade many research groups have focused on controlling the shape of inorganic nanostructures, [7][8][9][10][11][12] and many low-symmetry nanocrystals have been produced. [13][14][15][16][17][18][19][20] In this respect, one-dimensional structures are particularly interesting objects whose optical and catalytic properties strongly depend on their shape anisometry. [14][15][16][17] This unique feature of metallic nanorods has already found several applications in nanotechnology [21] and biomedical research. [22,23] Moreover, four examples of bimetallic nanorods [24][25][26][27] have been described in the last few years. It is believed that bimetallic platinum-on-gold and palladium-on-gold nanostructures may open a new direction in the area of catalysis. [28][29][30] However, all bimetallic nanorods reported to date are only soluble in water and therefore cannot catalyze any reactions in organic solvents. In fact, there are no examples of any platinum or palladium nanostructures covalently functionalized with polymer chains, which could render them soluble in organic media. Herein we describe the first example of polymer-functionalized platinum-on-gold nanostructures. We use gold nanorods as templates and demonstrate how a polycrystalline continuous shell of platinum can be deposited on their surface and subsequently functionalized with organic molecules. In addition, we provide conclusive evidence of the functionalization of the platinum shell by direct visualization of the polymer surface layer by electron microscopy and its detection by 1 H NMR spectroscopy.The seed-mediated method developed by Murphy and coworkers [1] and later modified by El-Sayed and Nikoobakht [2] produces single-crystalline gold nanorods (Au NRs). However, the conversion of Au I ions to Au 0 in this method is only 10-15 %, [31] and the majority of ions remains in solution after the growth of Au NRs is complete. Our systematic studies revealed that the amount of ascorbic acid used for the reduction of Au I ions is critically important, and addition of 10 mol % ascorbic acid after completed nanorod growth makes their size distribution much narrower. Figure 1 a shows a representative TEM image of Au NRs prepared by this modified method. The analysis of 250 nanorods shown in Figure 1 a revealed that their average length and width measure 52.8 and 11.4 nm, respectively, and the standard deviation (SD) for both dimensions is less than 9 %. These results represents a significant improvement in comparison with Au nanorods prepared under the standard conditions (SD % 20 %). [1,2] Further introduction of ascorbic acid allows conversion of Au I ions remaining in the growth solution into metallic gold and its deposition onto the surface of Au NRs.[32] However, this rapid addition of ascorbic acid results in a nonuniform deposition of gold, and the shape of the nanorods changes to...