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Although spectrally selective materials play a key role in existing and emerging solar thermal technologies, temperature‐related degradation currently limits their use to below 700 °C in vacuum and even lower temperatures in air. Here a solar‐transparent refractory aerogel that offers stable performance up to 800 °C in air is demonstrated, which is significantly greater than its silica counterpart. This improved stability is attributed to the formation of a refractory aluminum silicate phase, which is synthesized using a conformal single cycle of atomic layer deposition within the high‐aspect‐ratio pores of silica aerogels. Based on direct heat loss measurements, the transparent refractory aerogel achieves a receiver efficiency of 75% at 100 suns and an absorber temperature of 700 °C, which is a 5% improvement over the state of the art. Transparent refractory aerogels may find widespread applicability in solar thermal technologies by enabling the use of lower‐cost optical focusing systems and eliminating the need for highly evacuated receivers. In particular, a shift to higher operating temperatures while maintaining a high receiver efficiency can enable the use of advanced supercritical CO2 power cycles and ultimately translate to an ≈10% (absolute) improvement in solar‐to‐electrical conversion efficiency relative to existing linear concentrating systems. [ABSTRACT FROM AUTHOR]