Molecularly engineered materials obtained via the sequential combination of different nanomaterials is an encouraging methodological approach. Two-dimensional (2D) materials offer a platform that allows the construction of unique heterostructures with a diversity of physical and chemical properties. Most of the 2D heterostructures are composed of direct stacking of discrete monolayer fragments of individual materials. Although this method allows flexibility, it is sluggish, cumbersome, and mechanically weak. Instead, covalent functionalization provides stability and robustness to the heterostructure. GRAPHMOF is to elucidate the detailed structure of 2D MOF nanosheets covalently affixed with monolayer graphene and MoS2 using scanning probe microscopy. I will employ state-of-the-art scanning probe microscopy to unravel the nanoscale interfacial structure of 2D-2D heterostructures. The fundamental information obtained from the microscopy measurements will be employed to assess the influence of the heterostructures of the 2DMOF on either graphene and/or MoS2 electronic structure using Raman and PL spectroscopy. A clearer understanding and effective use of covalent bond formation could lead to the development of functional surfaces with potential applications in optoelectronic, supercapacitors and sensors. GRAPHMOF will allow me to pursue a highly innovative research line in surface science, providing me a perfect platform for my personal development in terms of research and training in a topic of key importance, i.e., 2D materials, direct covalent functionalization, and state-to-the-art imaging techniques. This project will also allow me to strengthen my teamwork and leadership skills as well as widen my scientific network and collaborations. In summary, this MSCA allowance will be a positive turning point in my academic career toward scientific excellence.