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Phenolic-metal complexation coatings have been discovered to be a universal route for the deposition of multifunctional coatings.However,most complexation coatings have been prepared by the immersion method,which limits their practical large-scale application.Herein,we describe a facile and green engineering strategy that involves spraying phenolic compound and metal ions on substrate to form in-situ complexation coating with different coordination states.The coating is formed within minutes and it can be achieved in large scale by the spray method.The pyrogallol-FeⅢ complexation coating is prepared at pH 7.5,which consists predominantly of bis coordination complexation with a small amount of tris-coordination complexation.It displays that the water contact angle is near zero due to the generation of rough hierarchical structures and massive hydroxyl groups.The superhydrophilic cotton resulting from the deposition of the pyrogalloI-FeⅢ complexation can separate oil/water mixtures and surfactant-stabilized oil-in-water emulsions with high separation efficiency.The formation of the phenolic-metal complexation coating by using spray technique constitutes a cost-effective and environmentally friendly,strategy with potential to be applied for large-scale surface engineering processes and green oil/water separation.