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ABX3‐type halide perovskite nanocrystals (NCs) have been a hot topic recently due to their fascinating optoelectronic properties. It has been demonstrated that A‐site ions have an impact on their photophysical and chemical properties, such as the optical band gap and chemical stability. The pursuit of halide perovskite materials with diverse A‐site species would deepen the understanding of the structure–property relationship of the perovskite family. In this work we have attempted to synthesize rubidium‐based perovskite NCs. We have discovered that the partial substitution of Rb+ by Cs+ help to stabilize the orthorhombic RbPbBr3 NCs at low temperature, which otherwise can only be obtained at high temperature. The inclusion of Cs+ into the RbPbBr3 lattice results in highly photoluminescent Rb1−xCsxPbBr3 NCs. With increasing amounts of Cs+, the band gaps of the Rb1−xCsxPbBr3 NCs decrease, leading to a redshift of the photoluminescence peak. Also, the Rb1−xCsxPbBr3 NCs (x=0.4) show good stability under ambient conditions. This work demonstrates the high structural flexibility and tunability of halide perovskite materials through an A‐site cation substitution strategy and sheds light on the optimization of perovskite materials for application in high‐performance optoelectronic devices. Adding stability: Lead halide perovskite nanocrystals (NCs) attract tremendous attention due to their extraordinary optical properties. Herein, we show that the partial substitution of Rb+ by Cs+ helps to stabilize the orthorhombic RbPbBr3 NCs at low temperature, which otherwise could only be obtained at high temperature (above 300 °C, see figure). [ABSTRACT FROM AUTHOR]