Metal halide perovskite semiconductors are excellent materials for next-generation solar cells. As a result of research and development all over the world, the photoelectric conversion efficiency for single-cell devices has rapidly improved to over 26% (as of July 2023), while the record efficiency for silicon-on-perovskite tandem devices currently stands at 33.7% (reported in May 2023). Materials chemistry has made many important contributions toward these remarkable results. In this account, we will introduce our achievements in these areas of material chemistry research for improving the performance of perovskite photovoltaics, including the development of high-purity precursor materials, and precursor inks tailored for large-area printed perovskite films. Studies of the nucleation and crystallization process, including simulations, have led to the reliable fabrication of high-quality perovskite films. Diverse new charge collection materials, as well as compounds to effectively modify the perovskite surfaces, have improved solar cell performance.