Heterogeneous material systems consisting of metallic structures and polymer matrixes are of significance for applications such as integrated circuits, microelectromechanical devices, antennas, sensors, actuators, and metamaterials. Scaly-foot snail which lives in the deep ocean exhibits high strength and temperature resistance due to unique shells made of metal and polymer. Recently, different multi-material structures have been fabricated with metal deposition using multiple manufacturing processes. However, using these complicated hybrid processes is challenging to construct complexthree-dimensional (3D) structures of heterogeneous material with enhanced properties, high resolution, and time efficiency. Here, we establish a novel manufacturing strategy to build bioinspired hierarchical structures with heterogeneous material systems using electrically assisted stereolithography. The photocurable printing solution that can act as an electrolyte for charge transfer was developed, and the curing characteristic of the printing solution was further investigated. A fundamental understanding of the formation mechanism of metallic structures on the polymer matrix was studied through physics-based multi-scale modeling and simulations. The correlation between metallic structures morphology, printing solution properties, and printing process parameters, and their effects in building bioinspired hierarchical structures with heterogeneous materials were identified. Demonstrative test cases were built to verify the printing performance of the proposed approach. This research work will deliver a scalable additive manufacturing (AM) process that can facilitate various interesting applications based on bioinspired heterogeneous material and structures.