Symmetry and pattern are precious forms of beauty that can be appreciated on both the macroscopic and molecular scales. Crystallographers have long appreciated the intimate connections between symmetry and molecular structure, reflected in their appreciation for the artwork of Escher. This admiration has been applied in the design of highly symmetrical coordination compounds. Two classes of materials are discussed: extended coordination arrays and discrete supramolecular assemblies. Extended coordination polymers have been implemented in gas separation and storage due to the remarkably porosity of these materials, aided by the ability to design ever-larger inner spaces within these frameworks. In the case of discrete symmetrical structures, defined inner and outer space present a unique aesthetic and chemical environment. The consequent host-guest chemistry and applications in catalysis are discussed.