Aberration-corrected STEM has become a standard analytical technique in the field of nanoscience. As “designer materials” have become more in demand in academic circles, verification of a desired product makes atomic-resolutionanalysis mandatory. Industry currently faces the same trend where tailor-made materials are customized for a given application. Here we show several examples where quantifiable atomic-scale manipulation of nanomaterials can have a dramatic impact on structure and, by extension, functionality.