Organic dyes have caused many negative effects on the aqueous environment and human health. Therefore, removal of organic dyes from water is a great challenge of seeking an effective methodology. Titanate‐based materials have been received much attraction and recognized as effective adsorbents for wastewater treatment. This study represented the feasibility of novel carbonaceous mesoporous titanate‐based materials (Na2Ti3O7/Na3Ti6O13) successfully synthesized via a EDTA‐Na2 assisted method to be used as adsorbents for removal of cationic dyes (methylene blue‐MB, and crystal violet‐CV). The samples synthesized with different molar ratios of EDTA‐Na2 (0.5, 1.0, 1.5 vs TiO2) were characterized by different analysis methods (SEM‐EDX, FT‐IR, XRD, BET and UV‐Vis). They were also tested for the treatment of both two dyes. Results showed that the sample with 1.0 EDTA‐Na2:1.0 TiO2 (MT1.0:1.0) had the highest and comparable removal efficiency for MB and CV among the as‐synthesized samples. The adsorption of both two dyes on MT1.0:1.0 followed the Langmuir isotherm with maximum adsorption capacities of 27.5 and 3.9 mg.g‐1 for MB and CV, respectively. It can also be found that the pseudo‐second‐order model showed the best fit with R2 values of 0.99 and 0.98 for MB and CV, respectively.