Electroless composite plating enables uniform and thin surface treatment along with composite deposition using nanoparticles. Among such particles, polytetrafluoroethylene (PTFE) is capable of dry lubrication because of its self-lubricating properties. Specifically, the PTFE content in a plating layer increases with the concentration of PTFE in the plating bath. However, a high concentration of PTFE interferes with the co-deposition of Ni and P, thereby reducing the plating speed. Additionally, PTFE is unevenly deposited on the surface of the plating layer. Consequently, a method for increasing the PTFE content at low PTFE concentrations is required. Therefore, in this study, a stirring process in a low-PTFE-concentration plating bath and a process wherein PTFE precipitates on a specimen without stirring were combined. The PTFE content of the plated layer deposited on high carbon steel, plated layer deposition rate, average friction co-efficient, static contact angle, and surface energy were evaluated as 25.96%, 3.44 µm/40 min, 0.195, 141.9°, and 2.74 mN/m, respectively. This technique prevented the decrease in the deposition rate of the plating layer and led to high PTFE content in the plating layer. Notably, even a thin plating layer (5 μm or less in thickness) showed excellent surface characteristics.