Illite-smectite (I-S) minerals from the Upper Jurassic oil-source shales of Denmark and the North Sea were studied by a complex of diffraction and spectroscopic methods. Detailed structures were identified to reveal the mechanism of postsedimentary transformations of these shales. Usually, oil is generated in the oil-source rocks of sedimentary basins simultaneously with the diagenetic and catagenetic I-S transformations. The results obtained demonstrate the relationship between these two reactions: NH3 molecules released from kerogen during the maximum oil formation are fixed as NH4 cations in smectite or vermiculite interlayers, forming mica or tobelite structural fragments. This solid-phase transformation produces the mixed-layer structures consisting of illite, tobelite, smectite, and vermiculite (I-T-S-V) layers.