In this paper, we adopted a novel method, namely, magnetron sputtering + low temperature ion sulfurizing composite technology to prepare synthetic MoS2/FeS multilayer film. The obtained film has a quite smooth surface with plenty of spherical particles. The friction tests were carried out on a ball-on-disc tester under dry condition. During the whole test, the friction coefficient of the MoS2/FeS multilayer film was always lower than that of the original 1045 steel and FeS film. In addition, the wear scar depth of the MoS2/FeS multilayer film was also low. It is undoubtedly that the synthetic MoS2/FeS multilayer film possesses excellent friction-reducing and wear-resisting behaviors.