When studying concrete impairment, the carbonation depth of concrete is regarded to be variable. Therefore, a time-varying reliability evaluation is important to perform a structural safety assessment. By analyzing 13,198 data on the carbonation depth of concrete, we propose a time-varying reliability evaluation based on the third-moment (TM) method to predict the service life of concrete. Validated by Monte Carlo (MC) simulation, the errors of the calculated results using time-varying reliability evaluation were within 4%. It is shown that the TM method proposed in this paper is more practical than traditional approaches such as MC simulation and second-moment (SM) methods in probability analysis. In this paper, exponential distribution was used to characterize the distribution of carbonation depths. Since paint was present on the concrete surface, numerous uncarbonized concrete components were found in the experiments; to develop a time-varying model considering the uncarbonized components, a function for evaluating the ratio of carbonized concretes is proposed. Overall, the time-varying TM method provided in this paper can act as a foundation for other investigations on probabilistic analysis, e.g., of compressive strength, deflection, and crack of concrete, which can be used to evaluate the reliability of concrete.