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Substituting a native ion in the crystals with a foreign ion that has a difference in valence, termed as aliovalent doping, has been widely attempted to upgrade solid-state ionic conductors for various charge carriers including O2−, H+, Li+, Na+, and so forth. 1− 4 The doping aids to promote the high-conductive framework and dredge the tunnel for fast ion transport. The garnet-type Li7La3Zr2O12 (LLZO) is a fast Li+ solid conductor, which received vast attention as an electrolyte candidate for allsolid-state lithium ion batteries, showing great potential to offer high energy density and minimize battery safety concerns to meet extensive applications in large energy storage systems such as electric vehicles and aerospace. 5− 8 In the Li-stuffed garnet framework of LLZO, the 3D pathway formed through the incompletely occupied tetrahedral sites bridged by a single octahedron enables the superior Li+ conductivity. 9, 10 For …