This paper presents an experimental study on the durability of adhesively bonded carbon fiber reinforced polymer (CFRP) – aluminum alloy single lap joints (SLJs) that are undergoing hygrothermal degradation. The failure loads of hygrothermally aged joints were measured and the corresponding fracture surfaces were investigated via visual observation and SEM. The variations of the Tg and the chemical components were determined by the DSC and FTIR analysis, respectively. The results demonstrate that the failure load of joints decreases nonlinearly as the aging duration increases, which approximates the exponential function. Cohesive failure is dominated before and after aging, meanwhile, the moisture absorption plasticizes the adhesive and leads to rougher fracture surfaces. The reduction in Tg and the FTIR results support the occurrence of a hydrolysis reaction in the adhesive due to hygrothermal aging. By quantitatively studying the relationship between the failure loads and the absorbance intensities of functional groups, a failure load prediction method was proposed. This method can establish the correspondence relationship between accelerated aging and actual service aging based on the chemical characteristics of adhesive, and realize the residual performance prediction of the bonding structure after hygrothermal aging rapidly and easily.