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Electrically actuated movement of liquid metals is quite promising in mechanical engineering and applied physics. However, little work has so far been performed on the effect of current polarity on the actuation of the eutectic gallium–indium (EGaIn) alloy moving on metal substrates. In this work, the spreading of EGaIn on copper (Cu) substrate under different direct-current (DC) polarities in the 0.5 mol/L NaOH solution was investigated, and the underlying mechanisms were addressed. When the Cu substrate was connected to cathode, the wetting was essentially attributed to the reduction in the oxidized surface of the Cu substrate; whereas, under the opposite polarity, the spreading was related to the tension gradient along the EGaIn–solution interface, which induced Marangoni flow, despite the fact that the EGaIn–Cu system was non-wetting in this case. Unlabelled Image • Application of DC drives the spreading of EGaIn on Cu substrate. • The spreading behavior varies greatly with DC polarity. • Spreading under wetting condition is primarily attributed to deoxidation of Cu surface. • Spreading under non-wetting condition is mainly due to Marangoni flow. [ABSTRACT FROM AUTHOR]