A vertical graphene heterostructure field-effect transistor (VGHFET) using an ultrathin ferroelectric film as a tunnel barrier is developed. The heterostructure is capable of providing new degrees of tunability and functionality via coupling between the ferroelectricity and the tunnel current of the VGHFET, which results in a high-performance device. The results pave the way for developing novel atomic-scale 2D heterostructures and devices.