Fires are always known for seriously deteriorating concrete in structures, especially for those with certain carbonation due to long-time service. In this paper, 75 prism specimens were prepared and divided into four groups (three carbonated groups and one uncarbonated group). Specimens were tested under different temperatures (20, 300, 400, 500, 600, and 700°C), exposure times (3, 4, and 6 hours), and cooling methods (water and natural cooling). Surface characteristics, weight loss rate, and residual mechanical properties (strength, initial elastic modulus, peak, and ultimate compressive strains) of carbonated concrete specimens after elevated temperatures were investigated and compared with that of the uncarbonated ones. Results show that the weight loss rates of the carbonated concrete specimens are slightly lower than that of the uncarbonated ones and that the cracks are increased with raising of temperatures. Surface colors of carbonated concrete are significantly changed, but they are not sensitive to cooling methods. Surface cracks can be evidently observed on carbonated specimens when temperature reaches 400°C. Residual compressive strength and initial elastic modulus of carbonated concrete after natural cooling are generally larger than those cooled by water. The peak and ultimate compressive strains of both carbonated and uncarbonated concrete specimens increase after heating, but the values of the latter are greater than that of the former. Finally, the constitutive equation to predict the compressive behaviors of carbonated concrete after high temperatures was established and validated by tests.