Due to low costs and exceptional photoelectric properties, perovskite solar cell materials have attracted great attention. During the fabrication of perovskite light-absorbing layers, dual-source vapor-deposited perovskite thin films suffer from long-standing issues of unknown growth mechanism and inferior crystallization quality, which negatively impacts the optical absorbance and charge carrier lifetimes of perovskite thin films, impeding the performance development of vapor-deposited perovskite solar cell devices. By utilizing bulky organic cations with different radii, this work designs quasi two-dimensional perovskite materials, and apply them as buffering templates at the perovskite/hole transport layer interfaces, thus manipulating the crystal growth process of vapor-deposited perovskite grains. The modified crystallization patterns result in vertically grown perovskite grains with columnar shapes, which notably enhances light-absorbing properties and carrier lifetimes of perovskite layers, boosting the power conversion efficiency from 16.21% to 19.55% on perovskite solar cells. The abovementioned results have provided valuable references to the vapor-deposited perovskite films and photovoltaic devices with outstanding optoelectronic performance.