By the introduction of an organic silane self-assembled monolayer, an interface-engineering approach is demonstrated for hole-conductor-free, fully printable mesoscopic perovskite solar cells based on a carbon counter electrode. The self-assembled silane monolayer is incorporated between the TiO2 and CH3NH3PbI3, resulting in optimized interface band alignments and enhanced charge lifetime. The average power conversion efficiency is improved from 9.6% to 11.7%, with a highest efficiency of 12.7%, for this low-cost perovskite solar cell.

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Additives are widely adopted for efficient, stable, and hysteresis‐free perovskite solar cells and play an important role in various breakthroughs of perovskite solar cells (PSCs). Herein the various additives adopted for PSCs are reviewed and their functioning mechanism and influence on device performance is described. The main roles of additives, modulating morphology of perovskite films, stabilizing phase of formamidinium (FA) and cesium (Cs)‐based perovskites, adjusting energy level alignment in PSCs, suppressing nonradiative recombination in perovskites, eliminating hysteresis, enhancing operational stability of PSCs, are summarized.