Cobalt nanoparticles (CoNPs) exhibit quite unique magnetic, catalytic, and optical properties. In this work, imidazolium-based ionic liquids (ILs) are successfully used to elaborate magnetically responsive suspensions of quite monodisperse CoNPs with diameters below 5 nm. The as-synthesized CoNPs adopt the noncompact and metastable structure of ϵ-Co that progressively evolves at room temperature toward the stable hexagonal close-packed allotrope of Co. Accordingly, magnetization curves are consistent with zero-valent Co. As expected in this size range, the CoNPs are superparamagnetic at room temperature. Their blocking temperature is found to depend on the size of the IL cation. The CoNPs produced in an IL with a large cation exhibit a very high anisotropy, attributed to an enhanced dipolar coupling of the NPs, even though a larger interparticle distance is observed in this IL. Finally, the presence of surface hydrides on the CoNPs is assessed and paves the way toward the synthesis for Co-based bimetallic NPs.