Compared with traditional centimeter-level electrodes, microelectrodes exhibit a small reaction area, high sensitivity, fast mass transfer rate, and low polarization current. However, current microelectrode preparation processes are very complicated and costly. Herein, we proposed a facile and universal method for fabricating single-particle microelectrodes. In the precursor solution, polyvinyl alcohol and ammonia were introduced as the polymeric binder and pore-forming agent, respectively. Through spaying-drying-sintering processes, the single-particle microelectrodes were successfully prepared for Li 4 Ti 5 O 12 (LTO), LiCrTiO 4 (LCTO), and LiFePO 4 /C (LFP/C), which showed excellent electrochemical properties. Furthermore, the single-particle microelectrode can be adopted to study the electrochemical oscillations of Li-ion batteries and assemble a full-cell microbattery as a potential next-generation microscale power source.