Abstract: Solid material NiSO4 was prepared. A TEACO2 laser generator was adopted as the light source to carry on laser stimulated surface coupling reaction of ethylene. The infrared vibration structure and adsorption state of C2H4adNiSO4 system were discussed based on infrared and temperature programmed desorption tests. It was showed that C2H4 is adsorbed as molecular state, bonding with NiSO4 surface through H atom at terminal O of S=O. The 1 079 cm－1 laser was selected to activate solid surfacial bond S=O, which absorbs the photon energy efficiently. At normal pressure and a temperature below 100 ℃, C2H4 conversed to butadiene with a high selectivity of 100％. Increasing laser pulse can improve conversion of C2H4 without change of selectivity. After 200 pulses, C2H4 in the system had been consumed to a large extent, and the product occupied most of the surface active sites, therefore conversion of C2H4 increased at a low speed. Temperature can also affect the laser stimulated surface reaction of C2H4adNiSO4. At 100 ℃, 15.1％ of C2H4 convert to butadiene, while keeping high selectivity of 100％. Based on the above experimental results, a mechanism of LSSR was proposed for the conversion of C2H4 to C4H6.