Carbon nanotubes (CNTs) have excellent performance, which means that they could be better electrical conductors. However, the problem of the connection of CNTs to electrodes limits their application. Particularly, improving connection efficiency while ensuring the quality of the connection is a big challenge, because it is difficult to form Ohmic contact between CNTs and electrodes. To address this issue, we propose the use of a femtosecond laser to irradiate the contact surface between the CNTs and the electrodes to obtain a good connection quality and electrical performance. At the same time, since the laser-induced connection acts on all the contact surfaces in the irradiation area, the connection efficiency can be improved, which provides a new idea for the large-scale preparation of the connection.