The growing interest in renewable energy sources has led to a significant focus on artificial photosynthesis as a means of converting solar energy into lucrative and energy‐dense carbonaceous fuels. First‐row transition metals have thus been brought to light in the search for efficient and high‐performance homogenous molecule catalysts that can accelerate energy transformation and reduce overpotentials during the catalytic process. Their dinuclear complexes have opportunities to enhance the efficiency and stability of these molecular catalysts, primarily for the hydrogen evolution reaction (HER) and water oxidation reaction (WOR). Recently, our group improved the catalytic activity, efficiencies, and stability of dinuclear molecular catalysts, particularly toward HER. Although one dinuclear complex has been tested for WOR, it demonstrated activity as water oxidation precatalysts. First‐row transition metals are a great option for sustainable catalysis because they are readily available, reasonably priced, and have multifaceted coordination chemistry. Examples of these metals are cobalt, copper, and manganese. The structure‐catalytic performance relationships of this first‐row transition metal‐based dinuclear catalysts are noteworthily interpreted in this account, providing avenues for optimizing their performance and advancing the development of sustainable and effective energy conversion technologies.