“…Nanomaterials with unique chemical and physical properties have wide promising application in catalysis, sensing, photography, optoelectronics, biomedicine, etc 1–6. During the preparation, multiparameters control is the key to achieve specific nanostructures, while a negligible parameter adjustment sometimes leads to fundamentally tremendous change in morphology of nanomaterial (e.g., size, shape, and composition), like the “butterfly effect.”7–10 Electrochemical deposition as a traditional nanomaterial preparation method has been widely employed to fabricate noble metal nanostructures via regulating multiple parameters including deposition time, potential, ion concentration, and temperature 11–13. However, traditional electrodeposition processes for new structure/function exploration are always carried out in large bulk solution system and usually surrounded by trial‐ and error‐based search, brute‐force enumeration, random selection, and intuition‐driven design,14–16 which lead to long research cycle, high reagent consuming/wasting and low efficiency and definitely hinder the fast paced advances in materials science today.…”