Vertical-axis wind turbines (VAWTs) are gaining attention for urban and offshore applications. However, their development is hindered by suboptimal power performance, primarily attributable to the complex aerodynamic characteristics of the blades. Flow control techniques are expected to regulate the flow on the blade surface and improve blade aerodynamics. In the present study, an effective active flow control technique, multiple boundary layer suction slots (MBLSS), is designed for VAWTs performance improvement. The impact of MBLSS on the aerodynamic performance of VAWTs is examined using high-fidelity computational fluid dynamics simulations. The response surface methodology is employed to identify the relatively optimal configuration of MBLSS. Three key parameters are considered, i.e., number of slots (n), distance between slots (d), and slot length (l), which vary from 2 to 4, 0.025c to 0.125c, and 0.025c to 0.075c, respectively. The results show that MBLSS positively affects the power performance and aerodynamics of VAWTs. Parameter n has the most significant effect on VAWT power performance and the importance of d and l is determined by tip speed ratios (TSRs). Tight and loose slot arrangements are recommended for high and low TSRs, respectively. The relatively optimal configuration (n = 2, d = 0.025c, l = 0.05c) results in a remarkable 31.02% increase in the average net power output of the studied TSRs. The flow control mechanism of MBLSS for VAWT blade boundary layer flow has also been further complemented. MBLSS can prevent the bursting of laminar separation bubbles and avoid the formation of dynamic stall vortices. This increases the blade lift-to-drag ratio and mitigates aerodynamic load fluctuations. The wake profiles of VAWTs with MBLSS are also investigated. This study would add value to the application of active flow control techniques for VAWTs.