Magnetic nanoparticles (MNPs) have shown exceptional potential for several biological and clinical applications. However, MNPs must be coated by a biocompatible shell for such applications. The aim of this study is to understand if and how the surface charge and coating can affect the electronic and magnetic properties of CoFe2O4 MNPs. The role of the surface on the total magnetic moment of MNPs is a controversial issue, and several effects can contribute to make it deviate from the bulk value, including the charge, the nature of the coating, and also the synthetic technique. Positively and negatively charged uncoated CoFe2O4 NPs as well as citrate-coated NPs were prepared by soft chemistry synthesis. The electronic properties and cationic distribution of CoFe2O4 NPs were probed by X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichroism (XMCD), and X-ray photoemission spectroscopy (XPS) techniques and confirmed by theoretical simulations. The overall magnetic behavior and the hyperthermic properties were evaluated by magnetometry and calorimetric measurements, respectively. The results show that all of the investigated CoFe2O4 NPs have high magnetic anisotropy energy, and the surface charge and coating do not influence appreciably their electronic and magnetic properties. In addition, the citrate shell improves the stability of the NPs in aqueous environment, making CoFe2O4 NPs suitable for biomedical applications.