Inorganic CsPbIBr2 perovskite features high phase stability and light absorption coefficient, making it suitable for the development of perovskite tandem cells or semi-transparent cells. High-quality CsPbIBr2 perovskite films are of crucial importance for fabricating efficient solar cells. However, compared with CsPbI2 and CsPbI2Br, the CsPbIBr2 precursor has poor crystallinity and low film coverage, which is prone to generating pinholes and defects. Therefore, serious charge recombination often occurs inside the devices. To solve this problem, p-aminobenzoic acid (PABA) is added to the CsPbIBr2 precursor to regulate its crystallization dynamics in this work. Electrostatic potential distribution of PABA shows that the electron-rich regions (negative charge regions) are mainly located near the C=O. Fourier transform infrared spectrum indicates the existence of coordination interaction between C=O and Pb²+ and the formation of hydrogen bonds between —NH2 and halide anions. Ultraviolet-visible absorption (UV-Vis) spectrum and X-ray diffraction (XRD) spectrum demonstrate that a new intermediate phase, PABA·Pb···Br(I), is formed between PABA molecules and the components of CsPbIBr2 precursor. The formation of this intermediate phase slows down the crystallization rate of the perovskite, regulates the grain growth, and enables the preparation of dense perovskite films. XRD, UV-Vis, space charge limited current, and linear sweep voltammetry are used to characterize the film quality. After the addition of PABA, the film quality of CsPbIBr2 perovskite is improved. Thus, the light absorption is enhanced. The defect density is reduced. And the conductivity is increased. The efficiency of the champion cell increases to 10.65% compared with that of the control cell (8.76%). Further, dark current-voltage curves, Mott-Schottky curves, electrochemical impedance spectra, and photoluminescence spectra are utilized to analyze the reasons for the improved photovoltaic performance. After the addition of PABA, the CsPbIBr2 device exhibits reduced leakage current, enhanced built-in electric field, suppressed charge recombination, and improved charge extraction at the interface. In addition to the enhancement in photovoltaic efficiency, the PABA-regulated perovskite cells also exhibit high stability. After being stored in air for 1500 h, the average efficiency of the unencapsulated cells remains 80% of the initial value.