Puzzles with chemicals echo a natural curiosity through our experiments with rocks, plastic blocks, and virtual objects in video games, revealing a deep-seated inclination to explore and master the microscopic world of atoms and molecules. Many of porous or macroscopic macromolecular structures even including bubble foams , not only crystalline materials, are known to belong Frank-Kasper (FK) phases which are puzzles of polyhedra fascinating intense study in various fields. Recent examples include the creation of materials from the FK phases, e.g., alloys , to macroscopic structures, e.g. functional polymers and large scale crystal engineering of DNA-assisted colloids .