Given the importance of positive impacts on the environment, it is necessary to evaluate the progress made thus far with water-splitting or electrocatalysis devices. Thus, this review aims to provide a broad picture of artificially developed hybrid materials, including organic (macro)molecules and perovskites, that can function in a synergistic manner and catalyze water-splitting events. This review highlights efficient hybrid organic-inorganic molecular systems integrated within an electrocatalysis device for the purpose of extracting energy from water, by splitting it in a cheaper way, with less energy input to initiate the pathway. The following review will highlight a large number of organic (macro)molecules, such as oligomers, polymers, and metal-organic frameworks, that have been introduced as tandem layers within a water-splitting device. The organic tandem layer is supposed to provide extra stability and enhance the photocatalytic activity. The review also discusses the drawbacks of existing devices based on hybrid organic-inorganic molecular systems to show what improvements are needed and what could be the future of these eco-friendly devices in a sustainable society on Earth and beyond.