Oriented single-domain magnetic nanoparticles with a high remanence ratio Mr/Ms and maximum magnetic energy product (BH)max have attracted immense attention. However, nanoparticles easily agglomerate due to their extremely small size, which impedes the process of orientation. So manipulating the orientation of nanoparticles is still a key challenge. Here, L10-FePt single-domain nanoparticles were successfully synthesized by a chemical method in the liquid phase and nanoparticle-based anisotropic nanocomposites were obtained by dispersing the nanoparticles in liquid epoxy resin under an external magnetic field. The main factors that impact the orientation of L10-FePt single-domain nanoparticles were investigated further. It is found that the dispersibility of nanoparticles has a great impact on the degree of orientation, so do the applied magnetic field and the concentration of nanoparticles. Nanocomposites with homodisperse nanoparticles oriented under a suitable external magnetic field exhibit excellent magnetic performance, such as high coercivity Hc and remanence Mr, which gives the nanocomposites a higher (BH)max than the isotropic samples. The anisotropic nanocomposites show great potential in multifarious permanent magnet applications and fundamental research.