Natural terrestrial radioactivity and cosmic ray ionization lead to the formation of air ions and charged aerosol particles even away from regions of active charge separation, such as in thunderstorms. The natural electrified state of the atmosphere has been studied for over a century; however, the effect of ionization on the physical properties of aerosols and clouds has rarely been studied in its own right except in thunderstorms. Here we review the status of our understanding of atmospheric charged particles and their influence on aerosol and cloud microphysical processes. We also review mechanisms that have been recently proposed to connect variations in the atmospheric ionization rate with variations in global cloudiness and weather systems. We conclude that a mechanism linking cosmic ray ionization and cloud properties cannot be excluded and that there are established electrical effects on aerosol and cloud microphysics. Necessary further work includes measurements of cloud, droplet, and aerosol charging and ion-aerosol conversion, together with modeling of the electrical aspects of nonthunderstorm cloud microphysics.