Hyperbranched polystyrenes (PS) were prepared by living radical photopolymerization of 4-vinylbenzyl N,N-diethyldithiocarbamate as an inimer under UV irradiation. The star-hyperbranched copolymers were derived by grafting from surface N,N-diethyldithiocarbamate groups of hyperbranched macroinitiator with t-butyl methacrylate in the presence of N,N-tetraethylthiuram disulfide. We obtained poly(methacrylic acid) star-hyperbranched PS nanospheres by hydrolysis of poly(t-butyl methacrylate)-grafted chains. We established two-dimensional (2D) regular nanopatterning by aligning continuously such nanospheres on poly(2-vinylpyridine) (P2VP) lamellar layers of PS-block-P2VP diblock copolymer film. Electrostatic interaction between nanosphere surface having negative charges (-COOCs) and P2VP lamellar layer acted effectively for the 2D nanopattern formation. (c) 2006 Wiley Periodicals, Inc.