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The presence of dyes and pharmaceuticals in natural waters is a growing concern worldwide. To address this issue, the potential of montmorillonite (MMT), an abundant clay in Colombia, was assessed for the first time for the removal of various dyes (indigo carmine (IC), congo red (CR), methylene blue (MB) and crystal violet (CV)) and pharmaceuticals (levofloxacin and diclofenac) from water. Initially, the MMT was characterized. TGA and FTIR showed OH groups and water adsorbed onto MMT. XRD showed an interlayer spacing of 11.09 Å and a BET surface area of 82.5 m²g⁻¹. SEM/EDS revealed a typical flake surface composed mainly of Si and O. Subsequently, the adsorbent capacity of MMT was evaluated for the removal of the pollutants. Adsorption isotherms showed a fit to the Langmuir model, which was confirmed by the Redlich–Peterson isotherm, indicating a monolayer-type adsorption. Furthermore, adsorption kinetics were best described by the pseudo-second-order model. Adsorption capacity (for dyes CV > MB > CR > IC) was associated with the attractive forces between the contaminants and MMT (PZC 2.6). Moreover, the findings evidenced that MMT can remove MB, CR, CV, and levofloxacin by electrostatic attractions and hydrogen bonding, while for IC and diclofenac only hydrogen bonding takes place. It was shown that MMT was most cost-effective at removing CV. Additionally, the material was able to be reused. Finally, the MMT efficiently removed CV in textile wastewater and levofloxacin in urine due to the positive charge of the pollutants and the low PZC of MMT.