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Thermal insulating materials are in high demand for heat flux regulation as they enhance energy conversion efficiency and reduce the consumption of fossil fuels. In this study, phase-reassembled high-entropy oxides (HEOs) were successfully produced via conventional solid-state reaction, and their thermophysical properties were investigated. Promising thermal barrier coating (TBC) candidates, A2B2O7and A3B′O7oxides, were reassembled to a single defective fluorite structure to further reduce the thermal conductivity via an entropy-stabilization strategy. The phase-reassembled HEO ceramics exhibited low thermal conductivity (1.06 W/m·K) and glass-like thermal conduction behavior owing to their highly distorted crystal structure. In addition, their compatible thermal expansion (∼9.95 × 10−6/K) suggests that the phase-reassembled HEOs are promising candidates for new thermal barrier materials. This study proposes a new strategy for reducing the thermal conductivity via phase reassemble beyond simply increasing the number of components.