Magnetite (Fe 3 O 4 ) particles have been electrochemically synthesized on self-supported carbon nanofiber (CNF) buckypaper. The Fe 3 O 4 crystals can be obtained by electrodeposition within a certain potential window with particle size controlled by the deposition time and confirmed by x-ray photoelectron spectroscopy (XPS), x-ray diffraction, and scanning electron microscopy (SEM). The magnetic properties of the Fe 3 O 4 buckypaper composite materials demonstrated a well-defined particle structure had been achieved. Electrochemical synthesis has been proven to be a cost-effective, high throughput, and highly efficient approach in fabricating Fe 3 O 4 /buckypaper composite nanostructures.