Abstract In this paper, we discuss the use of an electrospray method combined with a vapor-assisted solution technology (VAST) to prepare a perovskite solar cell absorber material. First, the PbI2 film was prepared using the electrospray method, and then through the VAST, the CH3NH3PbI3 perovskite absorber layer was formed, for which the device structure was ITO/PEDOT: PSS/CH3NH3PbI3/C60/BCP/Al. In the electrospray process, we changed the precursor solution concentration, voltage, and flow rate to control the thickness and surface morphology of the PbI2 film. In the VAST, we changed the CH3NH3I equivalent number and the heat treatment time, causing the CH3NH3I vapor deposited on the PbI2 film to form a CH3NH3PbI3 perovskite absorber layer. Finally, we completed the perovskite solar cell device. The power conversion efficiency (PCE) of the perovskite solar cell was 10.74%; the open circuit voltage (Voc) was 0.89 V; the short-circuit photocurrent (Jsc) was 21.30 mA/cm2, and the fill factor (FF) was 0.57.