Laboratory experiments simulating chemical aging of carbonaceous aerosol by atmospheric oxidants demonstrate that oxidative processing increases their ability to activate as cloud droplets. A microphysical model shows, however, that the measured increase in hygroscopicity is insufficient to lead to efficient wet scavenging for sub-100 nm particles that are typically emitted from combustion sources. The absence of an efficient atmospheric oxidation pathway for hydrophobic-to-hydrophilic conversion suggests that the fate of carbonaceous aerosol is instead controlled by its interaction with more hydrophilic species such as sulfates, nitrates, and secondary organic aerosol, leading to longer lifetimes, higher burdens, and greater contributions to climate forcing in the free troposphere than are currently estimated.