A review of the authors’ research works on Variable-Angle Spectroscopy (VASE) of graphene-based films is presented. The interaction of graphene oxide (GO) with magnetron-sputtered metals is a promising research area. VASE optical models of GO thin films deposited on magnetron-sputtered titanium (Ti), silver (Ag) and gold (Au) are discussed. Moreover, the optical properties of graphene nanoplatelet (GNPS) films and reduced graphene oxide (RGO) stabilized with Poly(Sodium 4-Styrenesulfonate) (PSS) films, which are less studied graphene-related materials, are shown. Finally, different optical behaviors of chemical vapor deposition (CVD)-grown monolayer, bilayer, and trilayer graphene films on silicon and polyethylene terephthalate (PET) substrates are recapitulated.