Abstract All‐inorganic α ‐phase CsPbI 3 perovskite with a suitable bandgap and superb optoelectronic properties is transforming the landscape of perovskite photovoltaics, but its long‐term lability associated with “soft” ionic lattice still imposes a great challenge for practical applications. Herein, a unique solid‐solution fluorination strategy is proposed to deliver an “ideal” perovskite matrix of α ‐phase CsPbI 3 abundant with F ions through interlocking the soft lattice of CsPbI 3 with cubic‐phase CsF·3/2HF. Such a sublattice interlocking can not only stabilize the soft lattice of α ‐phase CsPbI 3 perovskite nanocrystals but also passivate their notorious surface defects, thereby producing a “rigid” solid‐solution‐type perovskite/fluoride CsPbI 3 /CsF (termed as CsPbI 3 :F) nanocomposite with excellent long‐term stability and a near‐unity photoluminescence efficiency. Of particular note is that these CsPbI 3 :F nanocomposites can work well as effective grain boundary anchors to significantly improve the photovoltaic performance of perovskite solar cells because of their F‐rich perovskite lattice, achieving a T 80 stability of 1500 h under continuous maximum power point tracking and AM 1.5G illumination without the need for encapsulation. This work paves a new way to deliver perovskite materials with desirable properties for photovoltaics.