The controlled assembly in solution of gold nanocrystals modified by attachment of complementary protein-DNA conjugates is described. The size of the aggregates formed can be controlled by the addition of single-stranded DNA, which quickly terminates the assembly process. The rate of formation of the aggregates can also be controlled by varying the salt concentration. Consequently, two distinct regimes of aggregation kinetics are observed. At low salt concentrations, aggregation is shown to be dependent on the rate of duplex formation between the modified gold nanocrystals, i.e., reaction-limited. At higher salt concentrations, aggregation is shown to be dependent only on the rate of diffusion of the nanocrystals, i.e., diffusion-limited. The results presented provide important insights into the rates of formation of nanocrystal assemblies. Moreover, the approach adopted is modular, requiring only the relevant biotin linker chemistry to be developed for a given nanoparticle, while also precluding unfavorable interactions between the DNA and the streptavidin-coated nanoparticle. The ability to control the rate of formation and size of nanocrystal aggregates assembled is important new knowledge. Application of this knowledge will inform future studies of nanocrystal assembly in solution involving different types of nanocrystals, which is of increasing technological significance.