Extraordinary performance of natural supramolecular materials relies on combination of heterogeneous structures in 3D space. However, it is challenging to co-assemble building blocks with dramatically different physical/chemical properties in MSA. Hence, we have proposed a concept of “flexible spacing coating”, which has a highly compliant and flowable feature and is designated to pre-modify the building blocks beneath supramolecular groups. This flexible spacing coating could remarkably improve the molecular motility of the surface supramolecular groups, which favors for multivalency upon contacting of two macroscopic surfaces to realize assembly. Besides, the flowable and thick coating could compensate surface roughness of macroscopic building blocks to some degree, thus facilitating more groups reach interactive distance. Based on the flexible spacing coating, we have realized co-assembly of heterogeneous materials such as rubber/plastics, rubber/metal etc., thus to extend the applicable range of supramolecular assembly. Moreover, because of the flexibility of MSA in tailoring each building blocks, we have fabricated 3D ordered structures with diverse surface chemistry, leading to selective adsorption of fibroblast cells. We anticipated potential applications of this MSA methodology in constructing 3D microenvironment for tissue engineering.
