In 2005, the Science magazine, in commemorating the 125th anniversary of its founding, proposed 25 most challenging scientific issues in the future. One of the issues, "How far can we push chemical self-assembly?" has attracted the attention of scientists all over the world. During the 11th Five Year Plan period, NSFC convened scientists from various fields and proposed a major research project, "Controllable self-assembly system and its functionalization". Since the implementation of this project, Chinese scientists have developed and recognized a variety of noncovalent interactions, constructed numerous assembly building blocks with the "Chinese label", established a new assembly method similar to an organic "name reaction", realized the functions of multi-component and multi-level assemblies, and constructed a batch of controllable self-assembly systems having scientific importance and potential practical value. They have achieved great leap forward from following to original innovation, and brought the research of chemical self-assembly in China to move forward to the center of international stage. In this study, we examined the overall scientific goals, general layout of the plan, and ideas for implementation of the major research program "Controllable Self-Assembly System and its Functionalization", as well as an array of significant research accomplishments made possible through the funding received by the program.