Organic/inorganic nanohybrids hold great importance in fabricating multifunctional theranostics to integrate therapeutic functions with real-time imaging. Although Au nanorods (NRs) have been employed for theranostics, complicated design of materials limits their practical applications. In this work, new multifunctional theranostic agents are designed and synthesized employing Au NRs with desirable near-infrared absorbance as the cores. A facile "grafting-onto" approach is put forward to prepare the series of hierarchical nanohybrids (Au-PGEA and Au-PGED) of Au NRs and poly(glycidyl methacrylate)-based polycations. The resultant nanohybrids can be utilized as gene carriers with high gene transfection performances. The structural effect of polycations on gene transfection is investigated in detail, and Au-PGEA with abundant hydroxyl groups on the surface exhibits superior performance. Au-PGEA nanohybrids are further validated to possess remarkable capability of combined photothermal therapy (PTT) and gene therapy (GT) for complementary tumor treatment. Moreover, signifi cantly enhanced computed tomography (CT)/photoacoustic (PA) signals are detected both in vitro and in vivo, verifying the potential of Au-PGEA for dual-modal imaging with precise and accurate information. Therefore, these multifunctional nanohybrids fabricated from a simple and straightforward strategy are promising for in vivo dualmodal CT/PA imaging guided GT/PTT therapy with high antitumor effi cacy.advantage of both. [ 20,21 ] Particularly, a strategy was developed to functionalize Au NRs with poly(2-( N,N -dimethyl amino)ethyl methacrylate) (PDMAEMA) via "grafting-from" approach. [ 22,23 ] Although the as-prepared Au NRs exhibited great potential for GT and computed tomography (CT) imaging in vitro, the wellknown high cytotoxicity of PDMAEMA limits them for future clinical applications. Our recent study illustrates that compared with PDMAEMA, ethanolamine (EA) or ethylenediamine (ED)functionalized poly(glycidyl methacrylate) (PGMA) (denoted by BUCT-PGEA or PGED) exhibit lower cytotoxicity and superior gene transfection performances. [24][25][26] Besides the identical cationic pedant secondary amine and hydroxyl groups of PGEA, PGED also contains fl anking primary amine groups, [ 25 ] which allows tailoring the surface property of Au NRs through structural effects. These results inspire us to design Au NRs functionalized with PGMA-based polycations for theranostics.Herein, we exploit a facile preparation of organic/inorganic hierarchical nanohybrids based on PGEA-and PGED-modifi ed Au NRs for dual-modal imaging-guided combination of PTT/GT cancer treatment. It is noted that if the "grafting-from" strategy was applied, Au NRs would endure clustering and aggregation during preparation, resulting in loss of the NIR absorption property. In order to overcome this obstacle, the "grafting-onto" approach was put forward for the surface functionalization. In this regard, lipoic acid (LA) or lipoic acid anhydride (LA-LA) was successfully linked with PGEA...