This study introduces an innovative 3D-printed electrolyte with vertically aligned ion transport networks, containing well-dispersed nanoscale Ta-doped Li1.5Al0.5Ge1.5(PO4)3 (LLZO) in a poly(ethylene glycol) diacrylate (PEGDA) matrix. The 3DSE architecture, including spiral (s-3DSE) and pillared (p-3DSE) structures, enables efficient ion transport across the Li/electrolyte and electrolyte/cathode interfaces, enhancing active material mass loading and interfacial adhesion. The p-3DSE Li symmetric cell demonstrates a critical current density of 1.92 mA cm⁻² and stable operation for 2600 hours at room temperature. Full cells using p-3DSE achieve notable areal capacities of 2.75 mAh cm⁻² (LFP) and 3.92 mAh cm⁻² (NCM811). The optimized electrolyte structure provides superior mechanical properties and ionic conductivity, enhancing the overall stability of interfaces and improving the energy density of the entire cell.This study introduces an innovative 3D-printed electrolyte with vertically aligned ion transport networks, containing well-dispersed nanoscale Ta-doped Li1.5Al0.5Ge1.5(PO4)3 (LLZO) in a poly(ethylene glycol) diacrylate (PEGDA) matrix. The 3DSE architecture, including spiral (s-3DSE) and pillared (p-3DSE) structures, enables efficient ion transport across the Li/electrolyte and electrolyte/cathode interfaces, enhancing active material mass loading and interfacial adhesion. The p-3DSE Li symmetric cell demonstrates a critical current density of 1.92 mA cm⁻² and stable operation for 2600 hours at room temperature. Full cells using p-3DSE achieve notable areal capacities of 2.75 mAh cm⁻² (LFP) and 3.92 mAh cm⁻² (NCM811). The optimized electrolyte structure provides superior mechanical properties and ionic conductivity, enhancing the overall stability of interfaces and improving the energy density of the entire cell.