Moiré materials with flat electronic bands provide a highly controllable quantum system for studies of strong-correlation physics and topology. In particular, angle-aligned heterobilayers of semiconducting transition metal dichalcogenides with large band offset realize the single-band Hubbard model. Introduction of a new layer degree of freedom is expected to foster richer interactions, enabling Hund’s physics, interlayer exciton condensation and new superconducting pairing mechanisms to name a few. Here we report competing electronic states in twisted AB-homobilayer WSe2, which realizes a bilayer Hubbard model in the weak interlayer hopping limit for holes. By layer-polarizing holes via a perpendicular electric field, we observe a crossover from an excitonic insulator to a charge-transfer insulator at a hole density of ν = 1 (in units of moiré density), a transition from a paramagnetic to an antiferromagnetic charge-transfer insulator at ν = 2 and evidence for a layer-selective Mott insulator at 1 < ν < 2. The unique coupling of charge and spin to external electric and magnetic fields also manifests a giant magnetoelectric response. Our results establish a new solid-state simulator for the bilayer Hubbard model Hamiltonian. © 2022, The Author(s), under exclusive licence to Springer Nature Limited.