The use of collaborative robots (Cobots) for materials development in chemical laboratories is currently of high priority. Herein, the Cobot is used for autonomous continued analysis and synthesis of graphene oxide–polyethyleneimine‐based membrane to unify a method and prospects for big data collection are shown. Membranes have already demonstrated a selective affinity to potassium cations and promised to adjust permeability for other cations by changing pH. The Cobot allows a variation of membrane properties by its composition modification. The present strategy combines a novel perspective of material production by Cobots and the application of machine learning. Moreover, the current approach can be adapted for different modern chemical laboratories for various scientific research, and the proper workflow is provided.