Superparamagnetic nanoparticles (SPIONs) can be used as nuclear magnetic resonance (NMR) signal enhancement agents for petroleum exploration. This enhancement effect is uniform if SPIONs are monodisperse in size and in composition; yet it is challenging to synthesize mono disperse particles that do not aggregate in high salinity petroleum brine. Here, we report a method to synthesize individual SPIONs coated with tunable surface coating densities of poly(2-acrylamido-2-methyl-1-propanesulfonic acid (pAMPS) with a catechol end-group (pAMPS*). To establish parameters under which pAMPS*-coated SPIONS do not aggregate, we compared computational predictions with experimental results for variations in pAMPS* chain length and surface coverage. Using this combined theoretical and experimental approach, we show that singly dispersed SPIONs remained stabilized in petroleum brine for up to 75 h with high surface density pAMPS*.