A method of preparing an oxide-based solid electrolyte includes preparing a precursor solution which includes a lanthanide complex and a metal complex; preparing an intermediate by a hydrothermal reaction that is performed on the precursor solution; adding a lithium compound and a dopant precursor to the intermediate to prepare a mixture; and crystallizing the mixture. The mixture is crystallized by preparing a first oxide-based solid electrolyte by performing a first crystallization process on the mixture; and preparing a second oxide-based solid electrolyte by performing a second crystallization process on the first oxide-based solid electrolyte, wherein the second oxide-based solid electrolyte has a stoichiometric composition that is the same as that of the first oxide-based solid electrolyte, but that has a different crystal structure.