This paper describes a new strategy to generate nanocrystalline drugs through the precipitation of drug molecules in attoliter nanowells. We controlled the size of arsenic trioxide (ATO) nanocrystals by simply changing the concentration of ATO solution in the nanowells; particles with sizes ranging from 55 to 175 nm were formed. This approach only requires the drugs to be soluble in a solvent and thus can be broadly applicable to produce other drugs in nanocrystalline form.