For many applications, a polymer coating on nanocrystals is preferred over surface functionalization with small organic molecules or inorganic materials because the polymer coating increases repulsive forces between nanoparticles and improves their colloidal stability, preventing the formation of aggregates. This chapter provides an overview of some of the recent and, in the authors' opinion, more relevant methods for the synthesis of polymer–inorganic colloidal nanocomposites. Generally, both the inorganic and the polymer components can be prepared either independently (ex situ) or in the presence of the counterpart (in situ). The synthesis strategies are addressed in four main groups, corresponding to the four combinatorial possibilities. Furthermore, the most relevant covalent and non-covalent routes of functionalization of nanocrystals with synthetic polymers and biopolymers are reviewed.