There is a global problem with the effective purification of wastewater containing organic compounds, including dyes, pharmaceuticals and surfactants. Therefore, technologies for the removal of pollutants are still being explored. One of the promising methods could be the application of mineral sorbent composite based on lignite and bentonite. However, it is crucial to comprehensively recognize the mechanisms responsible for immobilizing organic compounds using mineral composite sorbents. The purpose of this work was to prepare and investigate the sorption mechanism of lignite-bentonite composite (BL) sorbents for the removal of dyes: Rhodamine B (RB), Remazol Brilliant Blue R (RBBR), pharmaceuticals: ibuprofen (IB), sulfamethoxazole (STX) and surfactant sodium dodecylbenzenesulfonate (SDBS). The quantitative sorption results have been performed using the high-performance liquid chromatography (HPLC) method. The application of infrared (IR) spectroscopy method was crucial to describe the sorption mechanism. After completing the sorption test, the spectra for the sorbents revealed bands associated with adsorbed RB, RBBR, IB, STX, and SDBS on the BL sorbent. Because lignite is predominated in BL composite, the sorption capacity and mechanism strictly correspond to its sorption properties rather than to bentonite ones. The spectra results indicate that the physical sorption process related to electrostatic forces, hydrogen bonding, and dispersion interactions are predominantly responsible for the immobilization of organic compounds tested on mineral sorbents. The X-ray diffraction (XRD) results indicate the ion exchange process involved in the case of RB adsorption on the bentonite sample. Nevertheless, the sorption mechanism was complex because of the extensive sorption properties of mineral composite and the different chemical properties of the tested organic compounds. The results of our spectroscopic studies help interpret the sorption mechanisms of organic compounds on mineral materials.