This paper provides an overview of our recent work in the area of bioinspired colloidal particles. We highlight how modifying the basic polyelectrolyte multilayer shell with materials such as light-absorbing gold nanoparticles, lipid bilayer membranes, and targeting ligands can functionalize colloids prepared the layer-by-layer assembly technique. These nanoengineered colloids are expected to show promise in areas ranging from drug and gene delivery to cell membrane modeling.