The disclosing of new diffusion frontiers for wind energy, like deep-water offshore applications or installations in urban environments, is putting new focus on Darrieus vertical-axis wind turbines (VAWTs). To partially fill the efficiency gap of these turbines, aerodynamic developments are still needed. This work in particular focuses on the development of a mathematical model that allows predicting the possible performance improvements enabled in a VAWT by application of the Gurney flaps (GFs) as a function of the blade thickness, the rotor solidity and geometry of the Gurney flap itself. The performance of airfoil with GFs was evaluated by means of detailed simulations making use of computational fluid dynamics (CFD). The accuracy of the CFD model was assessed against the results of a dedicated experimental study. In the simulations, a dedicated method to simulate cycles of variation of the angle of attack similar to those taking place in a cycloidal motion (rather than purely sinusoidal ones) was also developed. Based on the results from CFD, a multidimensional interpolation based on the radial basis functions was conducted in order to find the GF design solution that provides the highest efficiency for a given turbine in terms of airfoil and solidity. The results showed that, for the selected study cases based on symmetric airfoils, the GF positioned facing outwards from the turbine, which provides the upwind part of the revolution, can lead to power increments ranging from approximately 30% for the lower-solidity turbine up to 90% for the higher-solidity turbine. It was also shown that the introduction of a GF should be coupled with a re-optimization of the airfoil thickness to maximize the performance.