Coordination chemistry has always been the most important tool to envisage the material importance of metal–organic systems. The chemistry involved plays a key role in determining structural features, which are responsible for tuning the properties of materials. In the present review, the current trends of metal organic frameworks (MOFs), their structural properties and dye adsorption related to their structural architecture together with other parameters affecting adsorption phenomena are discussed. The content of hazardous dyes such as methylene blue, rhodamine B, and methyl orange has been continuously increasing in wastewater, and therefore, considering environmental safety, their removal is urgent. The present survey demonstrates the important role of MOFs in dye adsorption and separation. Their structure activity relationship, which is the most important factor, is elaborated through the current scenario. The mechanisms involved in the adsorption are also illustrated and explained. The mechanisms support that, besides the porous nature of MOFs, various non-covalent interactions also play a significant role in enhancing the adsorption of dyes. This review presents the modern trends of dye adsorption by MOFs and opens new doors for the further tuning of their structural features to modulate the adsorption/separation of hazardous materials, which will definitely guide the future endeavors of coordination chemists.