Inspired by the stimulation of biological systems， cyclic dipeptides self-assemble through the synergistic driving of various non-covalent interactions， such as hydrogen bonding and π-π stacking， to form functional materials with long-range ordered nanostructures， whose excellent physicochemical properties， such as unique photo-responsive properties and biocompatibility， have a wide range of applications in the fields of bio-photovoltaics and energy harvesting. In this paper， we focus on the structure-mechanism-function linkage of cyclic dipeptide self-assembly， and systematically illustrate its transition from basic research of molecular design to application. At the level of self-assembly mechanism， the entropy-driven crystallization dynamics is revealed， and the intermolecular forces and stacking arrangement are confirmed by crystallographic characterization techniques； at the level of functionality， the multi-dimensional applications of cyclic dipeptides as low-loss organic optical waveguide materials， piezoelectric sensors， and anti-bacterial and anticancer materials are analyzed. Through the establishment of non-covalent interaction network-microstructure-macroscopic performance constitutive model， we will point out the technical route for the development of biodegradable bioelectronic devices and intelligent drug delivery systems， and promote the cyclic dipeptide materials from basic research to the leapfrog development of precision medicine and flexible electronics industry.