Cementitious material specimens were immersed in a simulated acid rain solution for different time periods to allow deterioration to occur and then the specimen strengths were measured and the mineralogical compositions and microstructures were analyzed using Xray diffraction (XRD), Fourier Transform infrared (FT-IR) spectroscopy, scanning electron microscopy (SEM) and energy dispersive X-ray (EDX) diffraction. The simulated acid rain solution was prepared by mixing pure chemical reagents such as H2SO4, HNO3, MgSO4, and (NH4)(2)SO4. The experimental results show that the deterioration of cementitious material specimens under acid rain attack was mainly caused by the coupling of H+ and SO42-. In addition, simulated acid rain attack led to the gradual decomposition of cement hydration products such as Ca(OH)(2), calcium silicate (C-S-H) gel, xCaO center dot Al2O3 center dot yH(2)O (C(x)AH(y)) and ettringite followed by conversion to a white mushy mixture consisting of SiO2 center dot nH(2)O gel, Al2O3 center dot nH(2)O gel and CaSO4 center dot 2H(2)O but no AFt crystal, leading to the further deterioration of cementitious material specimens. The deterioration began from the exterior to the interior and continuously accumulated until the specimens were fully degraded. (C) 2012 Elsevier Ltd. All rights reserved.