Organic-inorganic hybrid perovskite as a kind of promising photovoltaic material is booming due to its low-cost, high defect tolerance, and easy fabrication, which result in the huge potential in industrial production. In the pursuit of high efficiency photovoltaic devices, high-quality absorbing layer is essential. Therefore, developing organic-inorganic hybrid perovskite thin films with good coverage, improved uniformity, and crystalline in a single pass deposition is of great concern in realizing good performance of perovskite thin-film solar cell. Here, it is found that the introduction of suitable amounts of LiI plays a dramatically positive role in enlarging the grain size and reducing the grain boundaries of absorbing layer. In addition, the carrier lifetime and built-in potential of the LiI doped perovskite device are observed to increase. Thus, it leads to about 15% gain in solar cell efficiency comparing to that without the LiI doping. Meanwhile, a hysteresis reduction is observed and 18.16% power conversion efficiency is achieved in LiI doped perovskite device, as well.