Acoustic emission (AE) and 4D X-ray computed tomography (4D XCT) were used simultaneously to study crack initiation and propagation in two different types of quartz-rich sandstones during the four-point bending experiments. Statistical analysis of the AE response indicated the failure mechanisms and their dynamics. The characteristic changes observed in the AE response defined the timing of the bending interruptions for XCT scanning to reveal the development of the crack. It was possible to quantitatively describe the developing cracks in their dimensions and volume and relate this information to the rate of decrease in the post-peak region of the material response. It could be concluded that the combination and concurrent use of AE and XCT techniques represents a highly effective and reliable instrument for observation, description, analysis of the crack propagation process, and rock disintegration in detail at a microscale level. With regard to the specific sandstones studied, Mšené sandstone is softer, respectively, less brittle, while Kocbeře sandstone is characterised by a more brittle behaviour accompanied by an AE signal with higher amplitudes compared to those of Mšené.