In summary, incorporating vertically aligned structures at the filler electrolyte interface exhibits excellent interfacial properties and ion transmission rate. This arrangement effectively avoids particle agglomeration caused by high surface energy ion migration along its vertical direction, facilitating the uniform deposition of Li⁺ on the metallic lithium anode. Additionally, the shortened lithium-ion conduction distance and excellent electrolyte/electrode interface contribute to enhancing the electrochemical performance of assembled solid-state batteries. By constructing vertically aligned fillers, it not only reduces interfacial impedance and increases ion diffusion, but also enables the preparation of flexible and stable CPEs.