We demonstrate a method for producing thickness- and refractive index-tunable antireflection coatings utilizing a one-step spin coating procedure with silica nanoparticle solutions. Aging nanoparticle solutions under controlled pH and temperature induces aggregation, allowing precise control of the porosity and refractive index of the spin-processed coating. Coating thickness measurements as a function of solution aging time and temperature allow for determination of the activation energy of the reaction-limited aggregation process. We demonstrate optimization of the antireflection effect for a single-layer silica nanoparticle coating on glass, and suggest that the aggregation method may be generalized to various other nanoparticle-based assemblies.