Synthesizing and assembling nanoscale building blocks to form anisotropic nanostnictures with the desired composition and property are of paramount importance for the understanding and use of nanostructured materials. Here we report a salt-tuned synthetic strategy using DNA-modified Au nanoparticles (DNA-AuNPs) to form Au-Ag head-body nanosnowman structures in >95% yield. We propose a mechanism for the formation of asymmetric Au-Ag nanosnowrnen from DNA-AuNPs, salts, and Ag-precursor-loaded polymers. Importantly, we show that oriented assemblies of various nanostructures are readily obtained using nanosnowmen with asymmetrically modified DNA as building blocks.