In this study, the effects of wind barriers on the crosswind environment of vehicle safety on a long-span bridge with a streamlined bridge deck were investigated at different angles of attack (AOA). The profiles of the mean and the root mean square (RMS) of the wind pressure coefficients above different traffic lanes were obtained through synchronous pressure measurements. The mean pressure fields around the bridge decks were investigated by computational fluid dynamics (CFD) simulations. The crosswind environment of vehicle safety between the deck with railings and the deck with wind barriers was compared and analyzed in detail at different AOA. The results showed that the wind barriers produce a thicker separation shear layer above the bridge deck and result in a larger negative pressure region in comparison with the case with railings. This leads to a notable reduction in the mean wind pressure coefficients above the deck. The increase in the AOA enhances the above-mentioned reduction effect. It was also found that the wind barriers significantly increase the RMS of the wind pressure coefficients above the deck compared with the railings. The increase in the AOA inhibits this enhancement effect. The results of the equivalent mean pressure coefficients show that the wind barriers reduce the vehicle sideslipping risk more effectively than the vehicle overturning risk. It was also found that the effect of the wind barriers on the reduction of the overturning risk is more sensitive to the change in AOA than the effect on the reduction of the vehicle sideslipping risk.