A method for aerosol-jet printing a layered perovskite structure by applying a PEDOT:PSS layer to a substrate; applying a layer of lead iodide (PbI2) to the PEDOT:PSS layer; and applying an aerosol mist of methylammonium iodide (CH3NH3I) atop the PbI2 layer with an aerosol-jet nozzle to form a CH3NH3PbI3 perovskite film layer. The substrate may be an ITO glass substrate, and the PEDOT:PSS layer may be applied by a process selected from spin-coating, inkjet-printing, slot-die-coating, aerosol-jet printing, physical vapor deposition, chemical vapor deposition, and electrochemical deposition. The PbI2 layer may be applied by a process selected from spin-coating, aerosol-jet printing, inkjet-printing, slot-die-coating, physical vapor deposition, chemical vapor deposition, and electrochemical deposition, and the PbI2 for application to the PEDOT:PSS layer may be in a solution of DMF, DMSO, γ-butyrolactone, or a combination thereof.