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The assembly of tiny magnetic particles in external magnetic fields is important for many applications ranging from data storage to medical technologies. The development of ever smaller magnetic structures is restricted by a size limit, where the particles are just barely magnetic. For such particles we report the discovery of a kind of solution assembly hitherto unobserved, to our knowledge. The fact that the assembly occurs in solution is very relevant for applications, where magnetic nanoparticles are either solutionprocessed or are used in liquid biological environments. Induced by an external magnetic field, nanocubes spontaneously assemble into 1D chains, 2D monolayer sheets, and large 3D cuboids with almost perfect internal ordering. The self-assembly of the nanocubes can be elucidated considering the dipole-dipole interaction of small superparamagnetic particles. Complex 3D geometrical arrangements of the nanodipoles are obtained under the assumption that the orientation of magnetization is freely adjustable within the superlattice and tends to minimize the binding energy. On that basis the magnetic moment of the cuboids can be explained.M agnetic particles show an intriguing self-assembly behavior, due to mutual magnetic interactions or interaction with external magnetic fields. This can already be experienced by playing with toy magnets, which can assemble into strings or clusters. For much smaller magnetic particles, the knowledge about the magnetic assembly is crucial for technical applications involving magnetorheological fluids (1), high-density magnetic storage devices, hyperthermal cancer therapy, and magnetic resonance imaging (2). These applications use small magnetic particles, in the micrometer size range for magnetorheological fluids and down to 10 nm for magnetic resonance imaging or magnetothermal cancer therapy. Decreasing the size of the particles further decreases their magnetic moment to an extent that they are not considered in those applications anymore. In consequence, the assembly of sub-15-nm magnetic nanoparticles has been scarcely explored (3). Only recently, it was reported that cube-shaped magnetic nanoparticles of 13 nm showed a surprising magnetic-field-induced assembly into helices at the air-liquid interface (4) and 9-nm magnetic nanoparticles in the presence of a magnetic field uniquely assembled into very large, nearly defectfree monolayers and 3D cubic assemblies on solid substrates (5). This triggers the question about the arrangement of the magnetic dipoles in such assemblies where an amazing answer was recently found in the case of only eight dipoles (6), and where for larger magnetic nanoparticles and their assemblies considerable complexity was observed (7, 8).Here we report very small (sub-15-nm diameter) spherical and cube-shaped iron-oxide nanoparticles with respect to their magnetic assembly behavior. The nanoparticles are sterically stabilized by oleic acid, have very narrow size distributions, and very regular shapes (SI Appendix). The controlled synthesis of...