Superparamagnetic carbon-coated Fe₃O₄ nanoparticles with high magnetization (85 emu·g^-1) and high crystallinity were synthesized using polyethylene glycol-4000 (PEG (4000)) as a carbon source. Fe₃O₄ water-based bilayer-surfactant-enveloped ferrofluids were subsequently prepared using sodium oleate and PEG (4000) as dispersants. Analyses using X-ray photoelectron spectroscopy, X-ray diffraction, and Fourier-transform infrared spectroscopy indicate that the Fe₃O₄ nanoparticles with a bilayer surfactant coating retain the inverse spinel-type structure and are successfully coated with sodium oleate and PEG (4000). Transmission electron microscopy, vibrating sample magnetometry, and particle-size analysis results indicate that the coated Fe₃O₄ nanoparticles also retain the good saturation magnetization of Fe₃O₄ (79.6 emu·g^-1) and that the particle size of the bilayer-surfactant-enveloped Fe₃O₄ nanoparticles is 42.97 nm, which is substantially smaller than that of the unmodified Fe₃O₄ nanoparticles (486.2 nm). UV–vis and zeta-potential analyses reveal that the ferrofluids does not agglomerate for 120 h at a concentration of 4 g·L^-1, which indicates that the ferrofluids are highly stable.