Poly(N-vinyl-2-pyrrolidone) (PVP)-coated Fe3O4 nanocrystals were prepared by a "one-pot" synthesis through the pyrolysis of ferric triacetylacetonate (Fe(acac)(3)) in N-vinyl-2-pyrrolidone (NVP). The polymerization of NVP was followed by measuring the shear viscosity of the reaction mixture. The PVP molecules formed in the reaction mixture was investigated by gel permeation chromatography. As the resultant Fe3O4 nanocrystals presented superdispersibility in 10 different types of organic solvents and aqueous solutions with different pH, including 0.01 M phosphate-buffered saline buffer, their hydrodynamic properties in both organic and aqueous systems were investigated by dynamic light-scattering. The results indicated that the PVP-coated Fe3O4 nanocrystals can completely be dispersed forming stable colloidal solutions in both organic solvents and water. Fourier transform infrared spectroscopy results suggested that PVP interacted with Fe3O4 via its carbonyl groups. Further surface analysis by X-ray photoelectron spectroscopy revealed that there were both coordinating and noncoordinating segments of PVP on the particle surfaced the molar ratio between them was of 1:2.6.