Polymers provide a useful tool for the controlled assembly of colloidal nanoparticles. We have developed a bricks and mortar strategy in which colloidal gold particles functionalized with recognition elements serve as the bricks and polymers bearing complementary functionality serve as mortar to hold together the nanoparticles. In this methodology, the conformational flexibility of the polymer compensates for irregularities in the size and shape of the aggregate structure. We have used this method to create discrete micrometer-scale spherical assemblies based on 2 nm gold nanoparticles. Both the size and shape of these assemblies can be controlled, providing spherical assemblies ranging from 50 nm to 1500 nm, as well as network structures.