The quantum Hall effect can be substantially affected by interfacial coupling between the host two-dimensional electron gases and the substrate, and has been predicted to give rise to exotic topological states. Yet the understanding of the underlying physics and the controllable engineering of this interaction remains challenging. Here we demonstrate the observation of an unusual quantum Hall effect, which differs markedly from that of the known picture, in graphene samples in contact with an antiferromagnetic insulator CrOCl equipped with dual gates. Two distinct quantum Hall phases are developed, with the Landau levels in monolayer graphene remaining intact at the conventional phase, but largely distorted for the interfacial-coupling phase. The latter quantum Hall phase is even present close to the absence of a magnetic field, with the consequential Landau quantization following a parabolic relation between the displacement field and the magnetic field. This characteristic prevails up to 100 K in a wide effective doping range from 0 to 1013 cm−2.

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The realization of graphene gapped states with large on/off ratios over wide doping ranges remains challenging. Here, we investigate heterostructures based on Bernal-stacked bilayer graphene (BLG) atop few-layered CrOCl, exhibiting an over-1-GΩ-resistance insulating state in a widely accessible gate voltage range. The insulating state could be switched into a metallic state with an on/off ratio up to 107 by applying an in-plane electric field, heating, or gating. We tentatively associate the observed behavior to the formation of a surface state in CrOCl under vertical electric fields, promoting electron–electron (e–e) interactions in BLG via long-range Coulomb coupling. Consequently, at the charge neutrality point, a crossover from single particle insulating behavior to an unconventional correlated insulator is enabled, below an onset temperature. We demonstrate the application of the insulating state for the realization of a logic inverter operating at low temperatures. Our findings pave the way for future engineering of quantum electronic states based on interfacial charge coupling.