The invention, relating to the field of battery production and energy storage, discloses a surface modification treatment method for increasing the activity of vanadium battery electrode materials, comprising the following steps: immersing a graphite-felt or carbon-felt material in a dispersion liquid of multi-walled carbon nanotubes for soaking, then cleaning, drying to obtain a modified graphite-felt or carbon-felt electrode material. According to the invention, mild and controllable surface modification treatment on the electrodes is carried out by using the multi-walled carbon nanotubes, the disadvantages of stability reduction of electrode materials and battery life shortening caused by peroxidation of the materials due to heat treatment and acid treatment are overcome, the technology is simple, and the cost is low. According to the invent, the graphite-felt or carbon-felt treated by the method as electrodes, a cation-exchange membrane as a separator, and positive and negative electrolytes which both consist of 1.5 M vanadyl sulfate and 2 M sulfuric acid form a battery, and the current efficiency, voltage efficiency, and energy efficiency of the battery are all obviously improved.