Biological particles may play an important role in the climate system by efficiently acting as ice nucleating particles (INPs) at a higher temperature range (e.g., above −20 °C where representative INPs such as mineral dust remain inactive), but there is an obvious lack of direct evidence that these particles serve in this manner. Here, we collected ambient particles under different weather conditions for identifying INPs that are active above −22 °C. The abundance of such efficient INPs increased during or following rainfall events. The extensive characterization of individual particles by three different analyses (particle morphology and composition, heat sensitivity of ice nucleation activities, and biological fingerprinting by DNA staining) revealed that efficient INPs have distinctly biological characteristics, which differ significantly from more abundant, representative, and relatively less active INPs, such as mineral dust. Additionally, by combining the heat-sensitivity experiments and DNA staining techniques, efficient INPs were found to contain heat-sensitive biomaterials and biological cells. Our findings provide direct evidence that biological particles are preferentially released into the atmosphere during rainfall events and act as important atmospheric INPs at higher temperature ranges (warmer than −22 °C), where typical INPs remain inactive.