Hybrid organometallic halide perovskite CH3NH3PbI2Br (or MAPbI(2)Br) nanosheets with a 1.8 eV band gap were prepared via a thermal decomposition process from a precursor containing PbI2, MABr, and MACI. The planar solar cell based on the compact layer of MAPbI(2)Br nanosheets exhibited 10% efficiency and a single-wavelength conversion efficiency of up to 86%. The crystal phase, optical absorption, film morphology, and thermogravimetric analysis studies indicate that the thermal decomposition process strongly depends on the composition of precursors. We find that MACl functions as a glue or soft template to control the initial formation of a solid solution with the main MAPbI(2)Br precursor components (i.e., PbI2 and MABr). The subsequent thermal decomposition process controls the morphology/surface coverage of perovskite films on the planar substrate and strongly affects the device characteristics.