Self-assembled dual-working electrode electrolytic cells were designed to produce twin alumina-Co composite films with highly symmetrical microstructures using a deflected electric field-assisted alternating current electrodeposition method. The results show that the deposition current density, microstructure, and optical and magnetic properties of the twin composite films exhibit a high degree of symmetry. The distribution of magnetic Co particles in the alumina nanopores can be changed by adjusting the magnitude of the deflected electric field, resulting in a synchronous symmetrical change in the microstructure of the composite films, which enables the fine-tuning of the magneto-optical properties of the twin alumina-Co composite films at the microscopic scale. The current density distribution on the surface of the twin composite films along the direction of the deflected electric field was quantitatively analyzed by theoretical calculations and numerical simulations. The results show that the deposition current density gradually increases from 0.024 A/m2 in region C to 0.056 A/m2 in region A at 6 V deflection voltage. The saturation magnetization intensity gradually increases along the radial direction, which is 118, 130, and 150 kA/m, respectively.