The clarification of the critical operating conditions and the failure mechanism of superlubricity systems is of great significance for seeking appropriate applications in industry. In this work, the superlubricity region of 1,3-diketone oil EPND (1-(4-ethyl phenyl) nonane-1,3-dione) on steel surfaces was identified by performing a series of ball-on-disk rotation friction tests under various normal loads (3.5–64 N) and sliding velocities (100–600 mm/s). The result shows that beyond certain loads or velocities superlubricity failed to be reached due to the following negative effects: (1) Under low load (≤ 3.5 N), insufficient running-in could not ensure good asperity level conformity between the upper and lower surfaces; (2) the high load (≥ 64 N) produced excessive wear and big debris; (3) at low velocity (≤ 100 mm/s), the weak hydrodynamic effect and the generated debris deteriorated the lubrication performance; (4) at high velocity (≥ 500 mm/s), oil migration occurred and resulted in oil starvation. In order to expand the load and velocity boundaries of the superlubricity region, an optimized running-in method was proposed to avoid the above negative effects. By initially operating a running-in process under a suitable combination of load and velocity (e.g. 16 N and 300 mm/s) and then switching to the target certain higher or lower load/velocity (e.g. 100 N), the superlubricity region could break through its original boundaries. The result of this work suggests that oil-based superlubricity of 1,3-diketone is a promising solution to friction reduction under suitable operating conditions especially using a well-designed running-in strategy.