At the University of Chicago MRSEC, Park and Sibener developed a synthesis of two-dimensional (2D) polymers with wafer-scale homogeneity, one monolayer thick, using a general and scalable growth method called laminar assembly polymerization. The lattice structures and optical properties of these freestanding crystalline films are directly controlled by altering the molecular monomers and polymerization chemistries. Because these 2D polymers are fully compatible with existing large-scale patterning and integration methods, a new powerful approach for interface engineering between dissimilar 2D building blocks has been identified. To demonstrate this, we successfully produced arrays of hybrid heterostructures and superlattices built layer by layer using 2D polymers and 2D atomic crystals based on MoS2.