This study explores the use of Halloysite NanoTubes (HNTs) as photocatalysts capable of decomposing organic dyes under exposure to visible or ultraviolet light. Through a systematic series of photocatalytic experiments, we unveil that the photodegradation of Rhodamine B, used as a model cationic dye, is significantly accelerated in the presence of HNTs. We observe that the extent of RhB photocatalytic degradation in 100 min in the presence of the HNTs is ~four times higher compared to that of bare RhB. Moreover, under optimized conditions, the as-extracted photodegradation rate of RhB (~0.0022 min−1) is comparable to that of the previously reported work on the photodegradation of RhB in the presence of tubular nanostructures. A parallel effect is observed for anionic Coumarin photodegradation, albeit less efficiently. Our analysis attributes this discrepancy to the distinct charge states of the two dyes, influencing their attachment sites on HNTs. Cationic Rhodamine B molecules preferentially attach to the outer surface of HNTs, while anionic Coumarin molecules tend to attach to the inner surface. By leveraging the unique properties of HNTs, a family of naturally occurring nanotube structures, this research offers valuable insights for optimizing photocatalytic systems in the pursuit of effective and eco-friendly solutions for environmental remediation.