Doping nature of MoSe₂, one of the promising Graphene analogous device material, can be tuned by controlling the concentration of functional groups in Graphene oxide (GO)@MoSe₂ heterostructure. In this study, by first-principles simulation, we have observed that GO can be used as a carrier injection layer for MoSe₂, where n or p type carriers are introduced within MoSe₂ layer depending on the type and concentration of functional moieties in it. Both n and p-type Schottky barrier height modulations are investigated for different modeled configurations of the heterostructure. This combinatorial heterostructure can be apromisingmaterial for future electronic device application.