This study aimed to create CTAB-modified bentonite organoclay (Bt@CTAB) by mixing the naturally occurring mineral bentonite (Bt) with the cationic surfactant cetyltrimethylammonium bromide (CTAB). Elemental analysis, N2 adsorption–desorption isotherm, scanning electron microscopy (SEM), FTIR spectroscopy, XRD, and thermogravimetric (TGA) analysis have been employed to analyze both the unmodified Bt and the Bt@CTAB organoclay. The dye sorption onto Bt@CTAB organoclay was investigated in the batch and column modes using aqueous solutions of anionic food dyes, viz., Sunset yellow FCF (E110), Azorubine (E122), and Ponceau 4R (E124) (individually or in a mixture). Experimental variables affecting the adsorption process, such as initial dye concentration, contact time, temperature, pH, and adsorbent dose, are evaluated. From the kinetic investigations, the adsorption of E110, E122, and E124 dyes well matched the pseudo-second-order kinetic model. E110 and E122 dyes adsorption onto Bt@CTAB attained equilibrium in 120 min while attained in 240 min for E124. The investigated food dyes were expected to achieve maximum adsorption efficiencies at concentration of 100 ppm of (E110 and E124) and 150 ppm of (E124), an adsorbent dosage of 0.4 gL−1, and an initial pH 5. In addition, Langmuir model best fits the sorption isotherm data, with the maximum adsorption capacity at 303 K being 238 mg/g, 248.75 mg/g, and 358.25 mg/g for E110, E122, and E124, respectively. The Bt@CTAB organoclay can be regenerated up to the 4th cycle successfully. The thermodynamic studies revealed the spontaneous and exothermic nature of the adsorption of these anionic dyes onto Bt@CTAB organoclay. The prepared cationic Bt@CTAB organoclay was successfully applied for the removal of E110, E122, and E124 from real water samples, synthetic effluents, and colored soft drinks with a recovery (R%) higher than 95%. The plausible adsorption mechanism of E110, E122, and E124 onto Bt@CTAB organoclay is proposed to be due to electrostatic interaction and hydrogen bond formation. Finally, the present study shows that Bt@CTAB organoclay may be employed efficiently and effectively to remove anionic food dyes from a wide range of real water and colored soft drinks.