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Perovskite solar cells (PSCs) are considered to be a promising candidate for near‐space applications due to their high specific power, excellent radiation resistance, and compatibility with flexible substrates. Nevertheless, the low‐temperature cycles impose considerable challenges to their long‐term stability. Herein, the extremely low‐temperature photovoltaic process of PSCs is investigated and the effect mechanisms of PAN (Polyacrylonitrile) as an additive are revealed. It is found that the additive PAN regulates perovskite lattice stress and stabilizes perovskite lattice structure and thus retards perovskite phase transition at low temperatures. Moreover, the PAN improves perovskite dielectric properties and ion migration activation energy and effectively passivates perovskite defects at low temperatures. Therefore, the carrier transport/extraction/collection abilities at low temperatures are enhanced effectively by alleviating exciton effect and increasing dielectric screening effect. Benefiting from these positive effects of PAN, the PAN‐modified device achieves a maximum efficiency of 24.34% at 150K and maintains 72% of its initial value after 120 thermal cycles (290‐130K). Also, the PAN‐modified flexible devices exhibit excellent bending stability and thermal cycle stability. This study provides a deep insight into understanding the extremely low‐temperature photovoltaic behavior of PSCs and demonstrates the potentiality of PAN additive strategy for achieving efficient and stable PSCs at low temperatures. [ABSTRACT FROM AUTHOR]