Nanoscale magnets with characteristic dimensions in the range of 1–100 nm are important in several areas of nanoscience and technology. First, this length scale spans the typical important dimensions of exchange lengths and domain-wall widths, which means that significant control of magnetic properties can be obtained by varying grain or particle dimensions. Second, the nonequilibrium synthetic processes used for clusters, particles, and films, often lead to new real-space crystal structures with completely novel spin structures and magnetic properties. Third, a basic-science challenge in this class of matter involves the spin-polarized quantum mechanics of many-electron systems containing 10–10 000 atoms. Finally, the materials under study may have important future applications in high-density data storage, ultra-small spintronic devices, or high-energy magnetic materials. In this article, we discuss our recent work on novel Fe-Au nanoclusters, MnAu-Mn core-shell structures, and complex high-anisotropy Co-rich intermetallic compound clusters. We also present new results on Fe-based alloys including the magnetic properties of semiconducting FeSi2 nanoclusters and spin correlations in FeGe nanocluster films.