In this paper, we propose a simple procedure to obtain multi-walled carbon nanotubes (MWCNTs) decorated with TiO2–Ag nanoparticles (MWCNT–TiO2–Ag). The MWCNTs were decorated with TiO2–Ag via combined functionalization with –OH and –COOH groups and a polymer-wrapping technique using poly(allylamine)hydrochloride (PAH). TiO2-modified Ag nanoparticles were synthesized via the Pechini method using a mixture of acetylacetonate-modified titanium (IV) isopropoxide with silver nitrate (with Ag+/Ti4+ atomic ratios of 0.5%, 1.0%, 1.5%, 2.0%, and 2.5%) and L(+)-ascorbic acid as reducing agents. XRD analysis revealed the formation of nanocomposites containing CNT, anatase TiO2, and Ag. The presence of nanoparticles on the MWCNT surfaces was determined using TEM. The morphology of the TiO2–Ag nanoparticles on the MWCNT surfaces was also determined using TEM. UV–Vis investigations revealed that an increase in the ratio between Ag+ and Ti4+ decreased the band gap energy of the samples. The characteristic vibrations of the TiO2, Ag, and C atoms of the graphite were identified using Raman spectroscopy. The photocatalytic activity of the MWCNT–TiO2–Ag nanocomposite was assessed by examining the degradation of Allura Red (E129) aqueous solution under UV irradiation. The dye photodegradation process followed a pseudo-first-order kinetic with respect to the Langmuir–Hinshelwood reaction mechanism. The spin-trapping technique evidenced that •O2− was the main species generated responsible for the Allura Red degradation.