The development of new iron-or cobalt-rich permanent-magnet materials is of paramount importance in materials science and technology since high-performance materials based on Nd2Fe14B or FePt are extremely expensive or subject to limited rare-earth supplies. [1][2][3][4] Aside from phase-diagram considerations, this requires alloys with high magnetocrystalline anisotropy K1 and Curie temperature Tc. However, the range of alternative compounds with appreciable K1 and high Tc is limited, and the situation is often aggravated by their metastable nature and by the requirement of high-formation temperatures. [5][6][7][8][9][10][11][12] For example, two suitable candidates are Zr2Co11 and HfCo7, both crystallizing in noncubic structures, as necessary for high K1. However, the poor control over phase purity in traditionally prepared bulk alloys has an adverse effect on permanent magnetic properties. [7,8,11,12] The future development requires high-performance magnetic materials for applications ranging from home appliances to sophisticated microelectronics and environment-friendly technologies, such as hybrid vehicles and wind turbines. [1][2][3][4] Synthesis of magnetic materials in the form of nanoparticles smaller than 10 nm has emerged as an alternative method to stabilize traditional or new crystal structures. [13][14][15][16][17] Small nanoparticles having high anisotropies also are essential as building blocks for highenergy nanocomposite magnets to ensure effective exchange coupling. [17][18][19][20][21] Wet-chemical and conventional physical vapor-deposition methods often require annealing at high temperatures to obtain the desired high-anisotropy crystal structures. In fact, this annealing step has been an important issue in controlling the size-distribution, self-assembly, easyaxis alignment, and nanostructure, not only in permanent magnetism but also in magnetic recording and other areas. [17][18][19][21][22][23][24][25] Easy-axis alignment of nanoparticles is particularly important to obtain high-energy products in permanent magnets because the energy product is quadratic in the magnetization. The annealing process and the associated sintering can be avoided by fabricating directly ordered nanoparticles using nonequilibrium cluster deposition, and this method can also be used to align the easy axes prior to deposition. [14][15][16] Here we show the fabrication of novel Zr2Co11 permanent-magnet nanostructures in a single-step process using cluster-deposition method. Our structures are free of rare-earths and expensive Pt and exhibit record energy products for this class of materials.A Zr-Co composite target of the required stoichiometry is sputtered using a directcurrent magnetron discharge into a water-cooled gas-aggregation chamber. [15,16,26] The sputtered atoms gain sufficient energy via collisions with ions to form nanoparticles with high-anisotropy structures in the gas-aggregation chamber before deposition on substrates kept at room temperature in the deposition chamber. The Zr2Co11 nanoparticles are...