Carbon dots (CDs) have attracted increasing attention in applications such as bio-imaging,sensors,catalysis, and drug delivery.H owever,u nlike metallic and semiconductor nanoparticles,the transfer of CDs between polar and nonpolar phases is little understood. Ac lass of amine-terminated CDs is developed and their phase transfer behavior has been investigated. It is found that these CDs can reversibly transfer between aqueous and organic solvents by alternatively bubbling and removing CO 2 at atmospheric pressure.T he mechanism of such CO 2 -switched phase transfer involves reversible acid-base reaction of amine-terminated CDs with CO 2 and the reversible formation of hydrophilic ammonium salts.Byusing the CDs as catalysts,the phase transfer is applied in the Knoevenagel reaction for efficient homogeneous reaction, heterogeneous separation, and recycling of the catalysts.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.