The disclosure provides materials, apparatuses, and methods for making multilayer coatings with a high degree of efficiency and control. In some aspects, for example, coatings are described having multiple layers of nanoparticles and a polyelectrolyte, wherein the nanoparticles form tightly packed monolayers. The interface between monolayers may include polyelectrolyte material. One or more aspects of such monolayers and interfaces are controllable.