Understanding and controlling interlayer coupling in van der Waals (vdW) materials is crucial for engineering novel electronic phenomena, including correlated states, topological phases, and superconductivity. Twisted bilayer graphene (TBG) offers a highly tunable platform to explore how interlayer orientation and separation influence quantum transport and moiré physics. Here, we introduce a method for achieving precise, atomic-scale control of interlayer coupling in TBG using dual-gated devices separated by ultrathin, thickness-tunable hBN spacers. This approach enables systematic control of interlayer interactions, demonstrating that the critical displacement field required for electron-hole bilayer behavior decreases as the layer separation increases at a fixed twist angle. Remarkably, at small twist angles, moiré-related side peaks persist even when layers are separated by tetralayers of hBN (approximately 1.3 nm), indicating robust interlayer band hybridization. By combining atomic-layer-precise control of interlayer coupling with independent twist angle tunability, our platform opens new avenues for discovering novel moiré physics governed by engineered interlayer coupling and moiré patterns.