In the present study, the effect of Co addition on Pd is investigated. Pd/CNT and PdCo/CNT catalysts are prepared via the sodium borohydride (SBH, NaBH4) reduction method. The X-ray diffraction, transmission electron microscope, and inductively coupled plasma-mass spectrometry analyses are performed to characterize the PdCo(70-30)/CNT catalyst. These characterization results reveal that Pd/CNT and PdCo/CNT catalysts are prepared successfully. NaBH4 electrooxidation activities of PdCo/CNT catalysts are examined with electrochemical methods such as cyclic voltammetry, chronoamperometry, and electrochemical impedance spectroscopy. PdCo(70-30)/CNT catalyst has 11.52 mA/cm(2) specific activity, 477.18 m(2)/g electrochemical active surface area, and the best electrochemical stability. Pd is a promising catalyst for NaBH4 electrooxidation reaction.