This talk addresses some of my group’s research highlights on MOFs and other functional materials, whereby we take a curiosity-driven approach to structure and derive novel applications for MOF materials, dry liquids and polymer films. I will discuss coordination modulation of MOFs to tune crystal morphology to produce micro and nanoparticles as well as strategies to produce MOF grass, microflower and micro-mushroom structures for imparting omniphobicity to a surface. I will also explore ways to dynamically control MOF orientation within their composites, and to create non-close-packed pore arrays in polymer films in a one-step manner. Fabrication of complex microstructures for surface functionalization often requires lithographic techniques and specialized equipment. By exploiting physicochemical interactions at air/liquid/solid interfaces, in combination with simple processing methods and bench-top techniques, we can create typically difficult-to-access microstructures, and show the importance of chemistry at interfaces to a wide variety of materials.