Sm-Co bulk alloys have shown superior permanent-magnet properties, but research on Sm-Co nanoparticles is challenging because of the need to control particle size, size-distribution, crystalline ordering, and phase purity. In the present study, a cluster-deposition method was used to produce Sm-Co nanoparticles having desired crystal structures without the requirement of subsequent high-temperature thermal annealing. Poorly crystallized SmCo5 nanoparticles exhibit a low room-temperature coercivity of only 100 Oe, whereas crystalline SmCo5 and Sm2Co17 nanoparticles show room-temperature coercivities of 2000 and 750 Oe, respectively. The direct synthesis of Sm-Co nanoparticles having sizes of less than 10 nm and a high degree of atomic ordering is an important step toward creating nanoparticle building blocks for permanent-magnets and other significant applications.