Although some progress in plasma modification of PTFE surface has been made recently, its adhesion strength still needs to be further improved. In this work, the surface of PTFE sample was treated with two-step in-situ method. Firstly, PTFE surface was treated with the capacitively coupled Ar plasma to improve its mechanical interlocking performance; Then Ar+NH3+CH4 plasma was used to deposit a-CNx:H crosslinking layer on the PTFE surface to improve molecular bonding ability. After treatment, a high specific surface area of 2.20 and low F/C ratio of 0.32 were achieved on the PTFE surface. Its surface free energy was increased significantly and its maximum adhesion strength reached 77.1 N·10 mm−1, 56% higher than that of single-step Ar plasma treated sample and 32% higher than that of single-step Ar+CH4+NH3 plasma treated sample, respectively.