To explore and evaluate the capabilities of the engineered LLM-based agents, we opted alcohol oxidation to the corresponding aldehyde as the model transformation considering the prevalent presence of hydroxyl and carbonyl functional groups in the fine chemical and pharmaceutical compounds . In particular, the synthesis sustainability has been one of the key considerations of the future green chemistry. Compared to the hazardous oxidants used for alcohol oxidations, such as chromium(VI) compounds , Dess-Martin periodinane , pyridinium chlorochromate (PCC) , and manganese dioxide (MnO2) , molecular oxygen from air is a promising terminal oxidant due to its low cost and high atomic efficiency with minimal wastes generated . Moreover, the implementation of molecular oxygen as the oxidant could operate under milder conditions, thus tolerating sensitive functional groups and enabling improved selectivity in the oxidation of alcohols to aldehydes. Thus, we focused on the search, screening, optimization, and scaling-up of an aerobic alcohol oxidation protocol to demonstrate the key roles of LLM-based agents during such a typical synthesis development process, hoping to illustrate the potentials of LLM in the practical synthesis development beyond the existing chemistry-knowledge-oriented chatting.