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Solvent-free ceramic/polymer hybrid electrolytes integrating two different ceramic electrolytes, Ge4+ or Ti4+ phosphates, are prepared and their electrochemical behavior is analyzed for both lithium-ion and lithium-air batteries (LIB and LAB). Li(Al, Ge)2(PO4)3 can be a more effective lithium conducting phosphate composition for a hybrid electrolyte that delivers an enhanced ionic conductivity (∼0.364 mS cm−1 at 30 °C), high discharge capacity and stable cycle retention. The enhanced electrochemical behavior is likely due to the densely packed grain boundary structure between inorganic particles and suppression of lithium reduction with the help of Ge4+. The proposed compositional design of a solvent-free hybrid electrolyte will be a competitive one, which possessed a stable electrochemical behavior both in conventional LIBs and in LABs without any interfacial control during the cell assembly i.e., soaking liquid electrolytes and/or additional interlayer components.