Pt nanoparticles were successfully deposited on uncatalyzed carbon paper by the supercritical CO2 deposition (SCD) method using platinum (II) acetylacetonate as a precursor followed by thermal conversion. A full 24 factorial design (four factors, each with two levels) was used to investigate the main effect of four factors (deposition temperature, deposition time, reduction temperature, and reduction time) and the interaction effects between them. The morphological structures and surface properties of the Pt/carbon paper composite were analyzed by X-ray diffraction (XRD), scanning electron microscope (SEM)/energy-dispersive X-ray spectroscopy analyzer (EDS), and high-resolution transmission electron microscopy (HR-TEM). The results of the 24 factorial design showed that Pt loading on the substrate correlated significantly with deposition time, while Pt aggregation slightly increased with the thermal reduction temperature. Data obtained from both XRD and HR-TEM were in good agreement and showed that Pt nanoparticles were homogeneously dispersed on the substrate with diameters of 7.2–8.7 nm.