AbstractSurface plasmons in graphene provide a compelling strategy for advanced photonic technologies thanks to their tight confinement, fast response and tunability. Recent advances in the field of all-optical generation of graphene’s plasmons in planar waveguides offer a promising method for high-speed signal processing in nanoscale integrated optoelectronic devices. Here, we use two counter propagating frequency combs with temporally synchronized pulses to demonstrate deterministic all-optical generation and electrical control of multiple plasmon polaritons, excited via difference frequency generation (DFG). Electrical tuning of a hybrid graphene-fibre device offers a precise control over the DFG phase-matching, leading to tunable responses of the graphene’s plasmons at different frequencies across a broadband (0 ~ 50 THz) and provides a powerful tool for high-speed logic operations. Our results offer insights for plasmonics on hybrid photonic devices based on layered materials and pave the way to high-speed integrated optoelectronic computing circuits.