The aggregation behavior and phase separation of nanorod (NR)/nanoparticle (NP) nanoinclusions immersed in semiflexible polymer brushes (PBs) are investigated by using molecular dynamics simulations. A variety of phases are formed by varying the size ratio q=sigma(r)/sigma(p), where sigma(r) and sigma(p) are the diameters of NR and NPs, respectively, and the attractive interactions epsilon(M) between NR/NP nanoinclusions and PBs. Ordered structures of NRs surrounded by large NPs are observed for the small size ratio q, and a dispersed mixture phase appears for the moderate size ratio q at weak attractive interaction. Meanwhile, the crystallization of NRs occurs at strong attractive interaction for the large size ratio q and a main face-centered cubic (fcc) structure combined with a small amount of hexagonal-closed packed (hcp) structure is observed. This investigation can provide some insights into the self-assembly of complex nanoinclusions and promise a new approach for controlling the self-assemble behavior of NPs. (c) 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2014, 52, 299-309