Abstract: For nearly a century, studying cosmic-ray air showers has driven progress in our understanding of elementary particle physics. In this work, we revisit the production of millicharged particles in these atmospheric showers and provide new constraints for XENON1T and Super-Kamiokande and new sensitivity estimates of current and future detectors, such as JUNO. We discuss distinct search strategies, specifically studies of single-energy-deposition events, where one electron in the detector receives a relatively large energy transfer, as well as multiple-scattering events consisting of (at least) two relatively small energy depositions. We demonstrate that these atmospheric search strategies especially the multiple-scattering signature – provide significant room for improvement beyond existing searches, in a way that is complementary to anthropogenic, beam-based searches for MeV-GeV millicharged particles. Finally, we also discuss the implementation of a Monte Carlo simulation for millicharged particle detection in large-volume neutrino detectors, such as IceCube.