Functional materials featuring semiconductor-like behavior have attracted significant interest in photocatalysis due to their widespread applications. However, traditional materials, such as metal oxides, metal sulfides, metal phosphides, and perovskites, not only suffer from low surface area and limited stability but also from absorption in the UV region of the solar spectrum. In this context, metal-organic frameworks (MOFs) offer not only a large surface area but also robust and tailorable architectures. Our research group has pioneered the development of metalloligand-based MOFs to have better structural control of the resultant materials. The step-wise design strategy successfully controls the structural dimensionality and the functional aspect of the resultant MOFs by varying the linker groups a metalloligand offers and selecting both primary and secondary metal ions. Notably, such metalloligands absorb light in the visible region of the solar spectrum, allowing them to function as the light-harvesting unit (i.e., photosensitizer) in the resultant MOFs. As a result, such MOFs function as remarkable heterogeneous photocatalysts for various catalytic reactions, including selective oxidation of substrates and cross-coupling reactions. This talk will discuss a few selected molecular architectures that offer tunable band gaps for excellent light harvesting properties to achieve desirable photocatalytic reactions only using visible light, air, and water.