The effects of electro-pulse on microstructure and mechanical properties of Al-Cu-Mn-Zr-V alloy were investigated, and the ageing mechanism was analyzed. As the current density increases, the size and quantity of precipitates gradually transit from continuous aggregation to dispersion at grain boundaries, and the mechanical properties are improved. When the current density is 15 A·mm−2, the precipitates are smallest and the mechanical properties are best. The tensile strength is 443.5 MPa and the elongation is 8.1%, which are 51.7% and 42.1% higher than those of conventional ageing treatment, respectively. Once the current density exceeds 15 A·mm−2, the precipitates will increase again and gather at grain boundaries, and the mechanical properties also decrease. An additional electrical free energy arising from an electro-pulse provides thermodynamic and kinetic conditions for the ageing precipitation of second phases. The electro-pulse can enhance the ageing diffusion coefficient, being improved by 34 times for 15 A·mm−2. The electro-pulse improves the nucleation rate and decreases the critical nucleation radii of second phases. However, it also accelerates the grain growth, making the second phases become coarse. An electro-pulse with a current density of 15 A·mm−2 can rapidly nucleate the second phase at 463 K while the precipitates are relatively small after growth.