Shotcrete (sprayed concrete) differs from ordinary cast concrete through the application technique and the addition of set accelerators that promote immediate stiffening. The bond strength development between shotcrete and rock is an important property that depends on the texture of the rock, the type of accelerator, and application technique. This investigation focuses on the development of the microstructure in the interfacial transition zone (ITZ) and the strength of the bond at the shotcrete-hard rock boundary. The results show that the bond strength is related to the hydration process—that is, the strength gain of the shotcrete—and remains low before the acceleration period of the cement hydration. With a scanning electron microscope (SEM), it is possible to observe changes over time for the early development of the interfacial zone, both before and after proper cement hydration. Results from tests with wet-sprayed concrete on granite rock are presented. The test method—using both bond strength and the SEM to investigate the development of the microstructure at the ITZ—is interesting, but has to be more broadly examined. Different mixtures, accelerators, and rock types have to be used.