Interfaces of cementitious layers have widely existed in construction projects, and they are the weakest part of the whole building. In this article, laser scanning and ultrasonic pulse, splitting tensile, and semi-disc fracture tests were carried out to study the bonding performance of cementitious layers. Different performance metrics, such as splitting tensile bond strength, ultrasonic pulse velocity, and attenuation of first arrival, were used to evaluate the bonding characteristics of the concrete layers. The results revealed that the parameters of the interface curve decreased, and the mechanical properties of the interface became weaker with an increase of the interval time. The amplitude of the first wave was more sensitive to the presence of the interface than the ultrasonic pulse velocity. Finally, the relationships between the performance metrics were analyzed. The fracture toughness of model I and mode II was highly correlated with the parameters of the micromorphology of the layered concrete, and the correlation coefficient is not less than 0.9511. The fracture toughness of mode I was strongly related to the splitting tensile strength, with a correlation coefficient of not less than 0.9744. This study was useful for the future study of the mode I and I fracture performance, the morphology, and other physical properties of cementitious layers.