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Ultraporous Pd nanocrystals for electrocatalysis applications were fabricated using a direct electrodeposition method on three differing carbon supports: flexible carbon fiber paper (CFP), and CFP modified with either graphene oxide nanosheets or their chemically reduced forms using a simple spray coating technique. The electrocatalytic activity of these electrodes was investigated for the direct electro‐oxidation reaction of methanol in alkaline media. Pd deposited on the CFP modified with reduced graphene oxide (rGO) has excellent poisoning tolerance to carbonaceous species and a significantly better catalytic activity toward methanol oxidation than the other two catalyst support materials. Pd/rGO/CFP in 2.0 M CH3OH in 2.0 M NaOH yields a specific current density of 241 mAmg–1 cm–2 determined at the anodic oxidation peak. It is believed that the collaborative effects due to the three‐dimensional ultraporous Pd nanocrystals and fast electron transfer owing to high conductivity of rGO nanosheets play an important role in enhancing the catalytic performance of Pd/rGO/CFP toward methanol oxidation in alkali media.