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Abstract The development of all‐solid‐state Li‐ion batteries requires solid electrolyte materials with many desired properties, such as ionic conductivity, chemical and electrochemical stability, and mechanical durability. Computation‐guided materials design techniques are advantageous in designing and identifying new solid electrolytes that can simultaneously meet these requirements. In this joint computational and experimental study, a new family of fast lithium ion conductors, namely, LiTaSiO₅with sphene structure, are successfully identified, synthesized, and demonstrated using a novel computational design strategy. First‐principles computation predicts that Zr‐doped LiTaSiO₅sphene materials have fast Li diffusion, good phase stability, and poor electronic conductivity, which are ideal for solid electrolytes. Experiments confirm that Zr‐doped LiTaSiO₅sphene structure indeed exhibits encouraging ionic conductivity. The lithium diffusion mechanisms in this material are also investigated, indicating the sphene materials are 3D conductors with facile 1D diffusion along the [101] direction and additional cross‐channel migration. This study demonstrates a novel design strategy of activating fast Li ionic diffusion in lithium sphenes, a new materials family of superionic conductors.