Due to its high ionic conductivity and stability to lithium metal, Li6.4La3Zr1.4Ta0.6O12 (LLZTO), as an element-doped garnet-type LLZTO material, has become one of the most promising solid electrolyte materials. However, traditional processing technologies of LLZTO materials lack of structural diversity and complexity, and the processing cost is high, making it difficult to be widely used in industrial production. Here, three LLZTO ink formulations are presented which allow for direct ink writing to print complex, cellular 3D structures with an accuracy of 150 µm, including hexagonal honeycombs, triangles and log pile square structures. Based on their tailored rheological properties, such as high modulus G' > 105 Pa, high yield stress σ ≈ 1000 Pa and distinct shear thinning, the inks have excellent printing properties. Based on these inks, LLZTO materials can be printed with three-dimensional freely designable electrolyte structures using common DIW 3D printers.