A unique way of achieving controllable, pressure-induced charge transfer doping in the graphene/MoS2 heterostructure is proposed. The charge transfer causes an upward shift in the Dirac point with respect to Fermi level at a rate of 15.7 meV GPa−1 as a function of applied hydrostatic pressure, leading to heavy p-type doping in graphene. The doping was confirmed by I2D/IG measurements. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.