Information acquisition and analysis of oil reservoirs are one of the most challenging and scientifically demanding areas in the oil exploration industry. Herein, we report a single-step solvothermal method for the synthesis of highly-stable hydrophilic and hydrophobic superparamagnetic iron oxide nanoparticles (SPIONs) as T2-contrast agents for oil reservoir applications. Hydrophilic and hydrophobic characteristics on the surfaces of SPIONs were achieved using polyethylene glycol (PEG-400) and oleylamine (OLA) for water/oil phases of the reservoir, respectively. For comparison, uncoated SPIONs were also prepared by coprecipitation method using NH4OH as a reducing agent. Stability of hydrophilic SPIONs was monitored in deionized (DI) water and/or artificial seawater (ASW), while stability of hydrophobic SPIONs was investigated in model oil (cyclohexane-hexadecane 1:1). X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) profiles confirm the magnetite (Fe3O4) phase of synthesized nanoparticles (NPs). The presence of C−O (532.4 eV) and −NH2 (399.7 eV) in XPS spectra of N1s and O1s substantiate the surface functionalization of Fe3O4 NPs with PEG and OLA, respectively. Transmission electron microscopy (TEM) images demonstrate the spherical shape NPs having particle diameters 11.6 ± 1.4, 12.7 ± 2.2 and 9.1 ± 3.0 for PEG-Fe3O4, OLA-Fe3O4, and Fe3O4, respectively. NMR T2-relaxation measurements were performed first time by an acorn area analyzer to demonstrate meaningful results for targeted reservoir applications. The transversal relaxivity (r2) values for PEG-Fe3O4 (66.7 mM-1 s-1) and OLA-Fe3O4 (49.0 mM-1 s-1) were 2.07 and 1.53 times higher than Fe3O4 (32.2 mM-1 s-1) NPs, respectively. The observed (i) quenching of T2-relaxation signals with SPION concentration, (ii) excellent relaxivity properties due to their ultra-small size, and (iii) long-term stability in different media, suggest them to be promising T2contrast agents for oil reservoir applications.