An effective photocatalyst obtained from composite nanofibers CA/GO fabricated by electrospinning technique followed by chemical crosslinking surface modified TiO2 nanoparticles (NPs) was used for removing the organic dyes Indigo carmine (IC) and Methylene blue (MB) from an aqueous solution under UV irradiation light. The crystalline structure and morphologies of CA-GO/TiO2-NH2 composite nanofibers were characterized by SEM, TEM, XRD, and FTIR. The prepared CA-GO/TiO2-NH2 composite nanofibers displayed significantly enhanced photocatalytic activity for photodegradation the organic dyes IC and MB under UV irradiation after 150 and 250 min respectively. The pH value of the solution was studied from 2 to 8 and obtained results showed a clear improvement of photocatalytic activity at pH 2. The results indicated that the activated CA-GO/TiO2-NH2 composite nanofibers functioned as an adsorbent for the removal of IC and MB from aqueous solutions. In addition, the results showed a high adsorption capacity remain up to 65% after five consecutive capacity cycles.