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In recent years, hybrid organic-inorganic (HOI) materials have attracted massive attention as they combine the unique properties of organic and inorganic compounds. In this review, we focus on the formation of HOI materials and their electrochemical performance that can be controlled by microstructural design depending upon their chemical composition. This overview outlines the recent strategies of preparing HOI materials on metallic surface via wet-electrochemical systems, such as plasma electrolysis (PE) and dip chemical coating (DCC). The corresponding electrochemical behavior for short and long term exposures is also summarized.