A novel thin-film lithium-ion battery (LIB) which can be charged by the light irradiation was fabricated by molecular precursor method. The unprecedented, translucent thin-film LIB, fabricated on a fluorine-doped tin oxide pre-coated glass substrate, was attained by using the active materials, titania for anode and LiCoO 2 for cathode, respectively. The averaged potential at 2.04 V was observed by applying a constant current of 0.2 mA. Then, that at 1.82 V was detected after 60 s during the sequential self-discharge process. The charging voltage of the assembled battery was 1.38 V with irradiation of 1-sun, the self-discharge voltage was 1.37 V. Based on the calibration curve of the charging voltages over constant currents ranging from 0-1.0 mA, the detected value can be theoretically reduced to the charging operation by applying a constant current of approximately 60 μA. The charge and discharge of this device was stable voltage at least 30 cycles. The two-in-one device can simultaneously generate and store electricity from solar light, the renewable energy source, and may be applied in smart windows for distributed power system according to on-site demand.Keywords: Photovoltaic device; lithium-ion batteries; translucent; molecular precursor method; thin film.Distributed power generation using renewable energy sources, such as solar light, can efficiently supply electricity according to on-site demand. If the electrodes of lithium-ion batteries (LIBs), which are the dominant power sources for most portable electronics, could function as a solar cell, the storage device could provide electricity without an electric power supply.We recently reported a transparent thin-film device that can function as a LIB. The thin-film LIB was fabricated with Li 4 Ti 5 O 12 (LTO) for the anode and Li 3 Fe 2 (PO 4 ) 3 (LFP) for the cathode on a fluorine-doped tin oxide (FTO) pre-coated glass substrate, and an electrolytic solution dissolving LiPF 6 . A wet process known as the molecular precursor method (MPM) was used to fabricate the active material thin-films with thicknesses of 100 nm on the substrates. 1 In the charge/discharge cyclic test of the LIB assembled with these electrodes, the synchronous electrochromic reactions of the LTO were clearly observed during repeated operation. Therefore, the transparent thin-film LIB has many practical applications, such as monitoring electrochemical reactions and use in electrochromic windows.Zhang et al. reported that titania particles immobilized on an anodic electrode constitute an excellent candidate for LIB active materials because of their high safety, good capacity retention, and low self-discharge. 2 In fact, titania has excellent cyclability and chemical stability and negligible toxicity in LIBs. 3,4 Additionally, anatase nanotubes have also been characterised as active materials and have been shown to have electrochemical potentials of 1.5À1.7 V versus Li/Li þ . 5 Regarding the chemical fabrication of two-in-one LIBs, we are therefore interested in the photovoltaic nature of ...