This paper aims to provide an aerodynamic optimization procedure to improve the aerodynamic performance of single-layer spherical domes, by coupling the kriging surrogate model with computational fluid dynamics (CFD) and finite element analysis (FEA). Firstly, a series of wind tunnel tests on the mean pressures and wind-induced behavior of a single-layer spherical latticed shell, were carried out to investigate the effect of dome geometric parameters. Then, the Reynolds-averaged Navier-Stokes equations and RSM turbulence model were utilized for simulating the wind loads on spherical domes, and the numerical results are validated with experimental data. On this basis, the single-objective aerodynamic optimization of spherical domes based on ordinary kriging surrogates has been carried out to find out the optimal geometric parameters (rise/span and wall-height/span ratios). The objectives were minimizing the highest mean suction and the maximum vertical displacement, respectively. The optimization results showed that the optimal design of spherical domes exhibits a reasonable aerodynamic performance improvement compared with the near optimal solutions. In addition, the highest mean suction and the maximum vertical displacement can be reduced by decreasing the wall-height of the dome, and a good trade-off between the two objectives can be achieved by selecting suitable dome geometric parameters.