An antisolvent (iodobenzene, IB) was used to assist the formation of closely packed CH 3 NH 3 PbI 3 (MAPbI 3 ) thin films during the one-step spin-coating process using different volumes of IB. The morphological, structural, optical and excitonic properties of MAPbI 3 thin films were analyzed using a contact-mode atomic-force microscope, X-ray diffractometer, broadband absorbance spectrometer and optical microscope-based time-resolved photoluminescence spectrometer. The properties of the resultant MAPbI 3 thin films can be manipulated by using different IB volumes, which dominates the device performance of MAPbI 3 based photovoltaic cells. The experimental results show that the grain size (or particle size) of MAPbI 3 thin films influences the collection of photoexcited carriers and the contact at the 6,6-Phenyl C 61 butyric acid methyl ester (PCBM)/MAPbI 3 interface, thereby resulting in a trade-off between the fill factor (FF) and short-circuit current density (J SC ). In addition, it is predicted that the power conversion efficiency (PCE) can be further improved by increasing the crystallinity of the MAPbI 3 thin film while keeping the small grain size.