A carbon aerogel (CA)-assisted CdS nanocomposite was prepared by hydrothermal process and was investigated as a photocatalyst towards the photodegradation of methylene blue (MB) dye and colorless phenol under visible light irradiation (VLI). CdS have attracted wide attention due to their relatively narrow band gap for the visible light effect and the suitably negative potential of the conduction band (CB) edge for the neutralization of H⁺ ions. The obtained characterization results suggest that the CA-assisted CdS nanocomposite has enhanced photophysical properties, a more surface area, and the desired morphology at the nm scale. Under optimization, CdS CA 8% shows superior catalytic activity for degradation compared with other samples. The photocatalytic activities of the as-synthesized samples were examined under VLI through the MB and phenol degradation. Compared with pure CA and CdS, the CA (8%)-assisted CdS nanoparticles (NPs) offer significantly enhanced photocatalytic efficiency for MB and phenol. The mechanism of photocatalytic reaction was examined by adding various scavengers, and the results revealed that the holes generated in CA (8%)-assisted CdS NPs have a crucial impact on the visible light photocatalytic process. The improved photocatalytic degradation was due to the strong interaction between the CA and CdS NPs.