Here we report the chemical synthesis of cobalt aluminum oxide (CoAl2O4) nanoparticles by a non-aqueous sol-gel route. The one-pot procedure is carried out at mild temperatures (in the 150 to 300 °C range), and consists of the reaction between cobalt acetate and aluminium isopropoxide in benzyl alcohol. The resulting CoAl2O4 nanoparticles show an unusually low average size, between 2.5 and 6.2 nm, which can be controlled by the synthesis temperature. The colorimetric properties of the nanoparticles are also determined by the synthesis temperature and the characteristic blue color of CoAl2O4 pigments is achieved in samples prepared at T ≥ 200 °C. The nanoparticles are antiferromagnetically ordered below ∼27 K with an uncompensated configuration. The uncompensated moment shows the typical features of strongly interacting superparamagnetic nanoparticles and spin-glass systems.