The correlation between negative pulse and the black electrolyte properties of magnesium alloy micro-arc oxidation and the treated area was investigated by introducing a negative pulse electric field. The physical phase composition, microstructure, elemental distribution, and content of the coating were analyzed using X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS). The results showed that the introduction of negative pulses favored the generation of MgO and MgSiO3 contents in the coatings, and an increase in the MgO phase was found in the coatings formed in the failed electrolytes; the microporous size and microcracks of the coatings were gradually and significantly reduced; the average consumption of Cu ions was 0.0453 g/L·dm2, which is only 26% of that in the unipolar condition; the introduction of the negative pulses significantly improved the "anomalous consumption" of Cu ions. The introduction of negative pulse can significantly improve the "abnormal consumption" of copper ions, which is attributed to the change in the electric field by negative pulse, which makes the cathode-enriched Cu ions migrate to the anode and reduces the reduction and precipitation of Cu ions at the cathode.