Self‐Correction Strategy for Precise, Massive, and Parallel Macroscopic Supramolecular Assembly

Macroscopic supramolecular assembly (MSA) represents a new advancement in supramolecular chemistry involving building blocks with sizes beyond tens of micrometers associating through noncovalent interactions. MSA is established as a unique method to fabricate supramolecularly assembled materials by shortening the length scale between bulk materials and building blocks. However, improving the precise alignment during assembly to form orderly assembled structures remains a challenge. Although the pretreatment of building blocks can ameliorate order to a certain degree, defects or mismatching still exists, which limits the practical applications of MSA. Therefore, an iterative poststrategy is proposed, where self‐correction based on dynamic assembly/disassembly is applied to achieve precise, massive, and parallel assembly. The self‐correction process consists of two key steps: the identification of poorly ordered structures and the selective correction of these structures. This study develops a diffusion‐kinetics‐dependent disassembly to well identify the poorly aligned structures and correct these structures through iterations of disassembly/reassembly in a programmed fashion. Finally, a massive and parallel assembly of 100 precise dimers over eight iteration cycles is achieved, thus providing a powerful solution to the problem of processing insensitivity to errors in self‐assembly‐related methods.