Macroscopic supramolecular assembly plays a key role to bridge the fundamental researches on molecular recognition to the potential applications as supramolecular materials. However, the challenge remains to promote the research from soft hydrogel system to semirigid objects or building blocks. Herein, the concept of flexible spacing coating was employed to modify the model polydimethylsiloxane building blocks, and reversible macroscopic assembly was successfully realized through introducing highly directional, dynamic, and reversible coordinate interactions as driving forces. The driving force for the macroscopic assembly was confirmed by introducing highly competitive ethylene diamine tetra acetic acid solution as an orthodox system to disassemble the assembled blocks. Moreover, the coordinate interaction was further understood through unique in situ measurements of binding forces between building blocks during assembly process. This work of macroscopic supramolecular assembly provides an in situ visible platform, which is significant to clarify the highly fascinating and facile coordinate interactions on the macroscopic assembly behavior. To increase understanding of macroscopic assembly with flexible spacing coating, a fascinating noncovalent interaction that can be employed in macroscopic assembly is coordinate interactions. Selfassembly through coordinate interactions has emerged as a wellestablished methodology, and metal-ligand interactions have been employed in construction of metallosupramolecular structures very frequently. A variety of elaborate metallosupramolecules, from 2-dimensional polygons to 3-dimensional cages, prisms, and polyhedra,