Most binary superlattices created using DNA functionalization or other approaches rely on particle size differences to achieve compositional order and structural diversity. Here we study two-dimensional (2D) assembly of DNAfunctionalized micron-sized particles (DFPs), and employ a strategy that leverages the tunable disparity in interparticle interactions, and thus enthalpic driving forces, to open new avenues for design of binary superlattices that do not rely on the ability to tune particle size (i.e., entropic driving forces). Our strategy employs tailored blends of complementary strands of ssDNA to control interparticle interactions between micron-sized silica particles in a binary mixture to create compositionally diverse 2D lattices. We show that the particle arrangement can be further controlled by changing the stoichiometry of the binary mixture in certain cases. With this approach, we demonstrate the ability to program the particle assembly into square, pentagonal, and hexagonal lattices. In addition, different particle types can be compositionally ordered in square checkerboard and hexagonal -alternating string, honeycomb, and Kagome arrangements. The field of DNA-mediated particle assembly has undergone remarkable progress over recent years (1), owing, at least in part, to its potential as a powerful platform for rational, bottomup design and engineering of complex materials, and motivated by recent successful translations into applications as diverse as sensing (2), photonics (3), and catalysis. The growing number of synthetic pathways and design strategies to fabricate DNA-functionalized particles (DFPs) has led to the development of a diverse palette of tailorable building blocks from which to choose, comprised of particles of a wide range of inorganic to organic compositions, a near continuum of particle sizes spanning nanometers to micrometers, precise DNA sequence control and thus tailorable hybridization, diverse chemistries for DNA grafting/association, and fine tunability of the grafting density. (4)(5)(6) Accompanying this expanding diversity of building blocks has been a parallel development of specific to generalized design principles that have begun to link molecular-scale DFP function with mechanisms of assembly and the resulting uni-or multi-modal crystalline structures.To this end, the growing combination of theory, simulations, and experiments, has helped to overcome some of the challenges in the field. For example, re-entrant melting strategies (7,8) have been successfully developed to alleviate the very narrow temperature ranges for efficient crystallization of DFPs.The most common route to induce attraction between DFPs, and thus program their assembly, leverages the direct or indirect (i.e., with additional DNA linker strand) hybridization of complementary DNA strands tethered separately to two types of particles. Under suitable conditions in such systems, particles with complementary DNA functionality (i.e., 'unlike' particles) form attractive contacts among multiple strands of h...