The fabrication of highly efficient nonviral gene carriers with low cytotoxicity remains a challenge in gene therapy. This paper reports a facile strategy to combine the advantages of gold nanorods (Au NRs) and polycations through surface functionalization. Different Au NR carriers with a controlled amount of poly(2-(N,N-dimethyl amino)ethyl methacrylate) (PDAEMA) brushes could be readily synthesized via surface-initiated atom transfer radical polymerization to achieve optimized nanohybrids for gene transfection. The obtained gene carriers demonstrate much higher gene transfection efficiency and lower cytotoxicity compared with polyethylenimine (similar to 25 kDa, gold standard of nonviral gene vector) in both COS7 and HepG2 cell lines. In addition, the potential of the PDMAEMA-grafted Au NR carriers to be utilized as a computed tomography contrast agent for the imaging of cancer cells has also been investigated. This strategy may realize the gene therapy and real-time imaging within one nanostructure and facilitate biomedical applications. (C) 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.