A C/CdS/TiO2 composite was prepared by a calcination method using sodium alginate (SA) as a medium. Remarkably, two nano-photocatalysts, TiO2 and CdS, were formed onto the carbon-based materials during calcination. The as-prepared hybrid materials were characterized and analyzed by XRD, SEM, TEM, XPS, UV-vis DRS, and PL techniques. The results showed that the coating of SA on the CH4N2S surface decreased the volatilization of CH4N2S. The carbon-based materials can not only play the role of a bridge connecting CdS and TiO2 for the efficient absorption of UV light, but also promote the construction of Z-scheme heterojunctions. The prepared photocatalysts were used in simultaneous adsorption and photocatalysis processes for the removal of organic dyes (cationic yellow X-GL) from aqueous solutions. After 60 min of UV irradiation, the photocatalytic decolorization rate of cationic yellow X-GL in aqueous solutions by C/CdS/TiO2 composite could reach 97.02%, which was 27% higher than that of TiO2. The reason was mainly due to the synergistic effect including the interface enhancement effect of hierarchical structure and the separation efficiency of photogenerated carriers. Additionally, it showed good recyclability making a promising photocatalyst material for the degradation of textile dyes.