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Self-assembled binary nanocrystal superlattices (BNSLs) represent an important class of solid-state materials with potentially designed properties. In pursuit of widening the range of applications for binary superlattice materials, it is desirable to develop scalable assembly methods that enable high-quality BNSLs with tailored compositions, structures, and morphologies. Here, we report the gram-scale assembly of crystalline binary nanocrystal superparticles with high phase purity through an emulsion-based process. The structure of the resulting BNSL colloids can be tuned in a wide range (AB13, AlB2, MgZn2, NaCl, and CaCu5) by varying the size and/or number ratios of the two nanocrystal components. Access to large-scale, phase-pure BNSL colloids offers vast opportunities for investigating their physiochemical properties, as exemplified by AB13-type CoFe2O4–Fe3O4binary superparticles. Our results show that CoFe2O4–Fe3O4binary superparticles not only display enhanced magnetic coupling but also exhibit superior lithium-storage properties. The nonclosed-packed NC packing arrangements of AB13-type binary superparticles are found to play a key role in facilitating lithiation/delithiation kinetics and maintaining structural integrity during repeated cycling. Our work establishes the scalable assembly of high-quality BNSL colloids, which is beneficial for accelerating the exploration of multicomponent nanocrystal superlattices toward various applications.