We report the formation of inorganic-organic (IO) hybrid perovskite (C 6 H 9 C 2 H 4 NH 3 ) 2 PbI 4 hexagonal nanosheets, using anisotropically grown PbO hexagonal nanosheets as a parent material. In place of the conventional chemical synthesis route, the PbO hexagonal nanosheets have been synthesized by the bottom-up electrochemical deposition technique. Conversion of PbO into the desired hybrid material has been achieved by the intercalation of organic moieties into the alternate layers of inorganic networks. These hybrid structures have shown strong room-temperature excitonic emission at 518 nm.An extensive study has been performed to observe the deposition parameters responsible for the growth of a well-defined hexagonal nanosheet. High-resolution transmission electron microscope results confirmed the growth of single crystalline hexagonal nanosheets in (110) plane orientation. Investigation of the surface morphology, further verified the formation of nanosheets with a smooth surface having an average roughness of 2 nm. The study revealed that the anisotropic growth of nanosheets is a result of different growth rates of crystal faces associated with the crystal lattice. ; Tel: +91 11 26591326 † Electronic supplementary information (ESI) available: Fig. S1: cyclic voltammogram of electrolyte solution used for deposition and X-ray diffraction pattern of as-deposited PbO lm. Table S1 shows the percentage of elemental composition of PbO nanosheets given by EDX result. Fig. S2 shows the effect of pH and concentration of precursors in the deposition bath. Fig. S3 shows the growth of hexagonal nanosheets as a result of secondary nucleation on the substrate. Fig. S4 shows the white light confocal microscopic images of PbO hexagonal nanosheets and photoluminescence images of converted inorganic-organic perovskite nanosheets. See