We report on a simple and robust route to the spontaneous assembly of well-ordered magnetic nanoparticle superstructures by irreversible evaporation of a sessile single droplet of a mixture of a ferrofluid (FF) and a nonmagnetic fluid (NF). The resulting assembled superstructures are seen to form well-packed, vertically arranged columns with diameters of 5~0.7 μm, interparticle spacings of 9~2 μm, and heights of 1.3~3 μm. The assembled superstructures are strongly dependent on both the magnitude of magnetic field and the mixing ratio of the mixture. As the magnitude of the externally applied magnetic field and the mixing ratio of the mixture increase gradually, the size and interspacing of the magnetic nanoparticle aggregations decrease. Without an externally applied magnetic field, featureless patterns are observed for the γ-Fe3O4 nanoparticle aggregations. The proposed approach may lead to a versatile, cost-effective, fast, and scalable fabrication process based on the field-induced self-assembly of magnetic nanoparticles.