The preparation of nanoparticles and their targeted connection with other functional units is one key challenge in developing nanoscale devices. Herein, we report an experimental strategy toward the development of anisotropic nanoparticle architectures. Our approach is based on phase separation of binary mixed polymer brushes on gold nanoparticle surfaces leading to Janus-type structures, as revealed by scanning transmission electron microscopy and electron energy-loss spectroscopy and, additionally, corroborated by computer simulation. We show that such structures can be used for the site-selective functionalization with additional nanosized entities.