Nanoaggregates were prepared from five samples of poly [(2-ethylhexyl acrylate)-ran-(tert-butyl acrylate)]-block-poly(2-cinnamoyloxyethyl acrylate), P(EYA-LBA)-PCEA in block-selective solvents for P(EXA-tBA). The effect of varying diblock composition, block-selective solvent, and equilibrium temperature on the size and shape of the nanoaggregates formed was investigated. Nanospheres were obtained after the photo-crosslinking of the spherical nanoaggregates. The tBA groups in the corona of these nanospheres could be hydrolyzed to give P(EXA-tBA-AA), where AA denotes acrylic acid, with a controlled fraction of AA units. Nanospheres with low contents of AA groups in their corona disperse well in low-polarity solvents and bind effectively to stainless-steel surfaces.