In this study, we present an investigation on the growth of thin Mo2C crystals via chemical vapor deposition using CH4. Optical microscopy (OM), scanning electron microscopy (SEM), atomic force microscopy(AFM), and Raman spectroscopy studies show that the morphology and the thickness of Mo2C crystals are strongly affected by the impurities in the system, the thickness of the copper substrate, and the graphene presence on Cu surface prior to Mo2C formation. Our studies show that during the CVD process, orthorhombic Mo2C crystals grow along the [100] direction on two different regions: directly on Cu surface or on graphene covered regions. Mo2C crystals that form on graphene are found to be thinner and less defective compared to the ones formed on the Cu surface. This is attributed to graphene acting as an additional diffusion barrier for Mo atoms diffusing through the copper. In addition to the graphene beneath the Mo2C crystal, Raman studies indicate that graphene may grow also on top of the Mo2C crystal, forming a graphene/Mo2C/graphene sandwich structure which may offer interesting properties for electronic applications.