Although the α-phase of formamidinium lead iodide (FAPbI3) has a suitable bandgap for use in solar cells, it must be stabilized with additional cations. These compositions can adversely affect the bandgap and produce lattice strain that creates trap sites for charge carriers. Kim et al. found that substituting small, equimolar amounts of cesium and methylenediammonium cations for formamidinium reduced the lattice strain and trap densities. The enhancement in open-circuit voltage led to a certified power conversion efficiency of 24.4%, and encapsulated devices retained 90% of their initial efficiency after 400 hours of maximal power point operating conditions. Science, this issue p. 108 Doping of cesium and methylenediammonium for formamidinium cations decreased lattice strain and increased carrier lifetime. High-efficiency lead halide perovskite solar cells (PSCs) have been fabricated with α-phase formamidinium lead iodide (FAPbI3) stabilized with multiple cations. The alloyed cations greatly affect the bandgap, carrier dynamics, and stability, as well as lattice strain that creates unwanted carrier trap sites. We substituted cesium (Cs) and methylenediammonium (MDA) cations in FA sites of FAPbI3 and found that 0.03 mol fraction of both MDA and Cs cations lowered lattice strain, which increased carrier lifetime and reduced Urbach energy and defect concentration. The best-performing PSC exhibited power conversion efficiency >25% under 100 milliwatt per square centimeter AM 1.5G illumination (24.4% certified efficiency). Unencapsulated devices maintained >80% of their initial efficiency after 1300 hours in the dark at 85°C.