Conjugated polymer nanostructures (CPNs) emerge as a new class of photocatalysts for organic pollutant degradation under UV and visible light. Polyprrole (PPy), as a conjugated polymer, exhibits a wide range of applications. We present here the first demonstration of employing pure PPy nanostructures as a very efficient photocatalyst for water depollution. PPy nanostructures were synthesized in hexagonal mesophases (used as soft templates) by chemical polymerization (PPy-NS-c), obtained by radiolysis (PPy-NS-γ), and synthesized without any template via chemical method (PPy-bulk) as bulk. The different PPy samples were characterized by SEM, TEM, FTIR and UV-vis absorption spectroscopy. The photocatalytic activity of both PPy nanostructures (PPy-NSc and PPy-NS-γ), which remain very stable after several cycles, was evaluated for the degradation of organic pollutant in aqueous solution (phenol and methyl orange were taken as a model pollutant). PPy nanostructures show high photocatalytic activity under both UV and visible light while bulk PPy (PPy-bulk) has no appreciable activity. PPy-NS-c present the highest activity for photodegradation of phenol under UV light, while PPy-NS-γ exhibit the best photocatalytic activity under visible light. We demonstrate here that the nanostructuration of these polymers is an important factor for their application in photocatalysis.