In summary, we disclosed a primitive thioesterification/hydrolysis reaction cycle fueled by T3P. A comprehensive screening of reaction conditions was conducted, including variations in amino acid species, substrate concentrations, T3P amounts, and pH levels. The results demonstrated that the structure of precursor molecules plays an essential role in constructing ordered self-assembly aggregates in aqueous solutions. Various characterization techniques were employed to gain deeper insights into the reaction cycle. Notably, intriguing kinetic behaviors of OA-Phe-AcCA aggregates were observed through fluorescence microscopy, which enabled real-time monitoring of morphological changes. Further studies on mimicking different primitive chemical reactions are underway in our laboratory.