In the present work, the usefulness of cetyltrimethylammonium bromide-modified palm oil fiber (CTAB-modified POF) for the removal of indigo carmine (IC) and 2,6-dichlorophenolindophenol (2,6-DCPIP) from aqueous solutions was investigated. Raw, NaOH-treated, and CTAB-modified POF were characterized by Fourier-transform infrared (FT-IR) spectroscopy, elemental analysis, thermogravimetric-hyperdifferential scanning calorimetric (TG-HDSC) analysis, X-ray diffraction (XRD), and scanning electron microscopy (SEM). e adsorption studies of IC and 2,6-DCPIP were performed in batch mode using CTAB-modified POF. e results showed that equilibrium was attained after a contact time of 30 minutes for IC and 20 minutes for 2,6-DCPIP. e maximum capacity of adsorption was obtained at pH � 2. e capacity of adsorption considerably increased with modified biosorbents and with increasing initial concentration of dyes. e ionic strength favors the increasing adsorption capacity of IC and does not affect the adsorption capacity of 2,6-DCPIP. e percentage of adsorption increased with increasing mass of the biosorbents. e nonlinear regression of adsorption isotherms showed that Freundlich (r 2 � 0.953; χ 2 � 4.398) and Temkin (r 2 � 0.986; χ 2 � 1.196) isotherms are most appropriate to describe the adsorption of IC and 2,6-DCPIP on CTAB-modified POF, respectively. e maximum adsorption capacities determined by the Langmuir isotherm were 275.426 and 230.423 μmol·g − 1 for IC and 2,6-DCPIP, respectively. e linear regression of adsorption kinetics was best described by the pseudo-second-order model (R 2 ≥ 0.998). e diffusion mechanism showed that external mass transfer is the main rate controlling step. Desorption of the two dyes is favorable in the alkaline medium.