Quantum Hall effects (QHE) host one-dimensional topologically-protected edge channels, which can serve as an essential ingredient in exotic quantum electronic systems. Yet the manual reconstruction of Landau-level topology, by electrostatic confinement or symmetry breaking, remains experimentally challenging. Here, we show that interfacial charge transfer in between CrOCl and large-angle twisted bilayer graphene offsets the two otherwise decoupled Dirac Landau-level ladders in each graphene layer, creating a new sequence of composite filling configurations. At charge neutrality, the composited (+2,-2) state involves only the zeroth Landau levels and becomes fully insulating, with longitudinal resistance reaching the GΩ regime. By contrast, higher composite zero-filling quantum Hall states, including (+6,-6) and (+10,-10), retain counter-propagating helical edge channels and exhibit pronounced non-local transport, reaching up to 50% of the local response. We attribute such switching-behavior to the Landau-spinor Hilbert space – as the filling is reduced from (+6,-6) to (+2,-2), the orthogonal N=±1 orbital components are removed, eliminating the edge-compatible channel and gapping both bulk and boundary transport. The interaction nature of the observed gapped sates was further examined both experimentally and theoretically. Our results suggest that charge transfer provides a direct route to engineer artificial quantum Hall insulators, opening possibilities for wavefunction-selective control of helical edge modes.