Molded sisal fibers dip-coated with titanium dioxide (TiO2) nanoparticles were physico-chemical characterized and tested for the photocatalytic treatment of textile wastewaters. The X-Ray powder diffraction (XRD), X-Ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM) and the scanning electron microscopy (SEM) analysis revealed uniform TiO2 nanoparticles deposition in the anatase phase with and average diameter of 32 nm. The sisal/TiO2 nanocomposite exhibits a remarkable photodegradation yield of methylene blue solution (92%) maintaining a good efficiency even after 5 washing cycles (70%). The nanocomposite also exhibits a remarkable fast photo-induced hydrophilicity decreasing the contact angle from 140° to 6° after 7 minutes of UV exposure. Sisal fibers revealed to be a promising substrate for TiO2 nanocomposites in wastewater treatment due to its low cost, low density, high specific strength and modulus, no health risk, easy availability and renewability.