Exchanged clays and cross-linked algae were compared based on their properties for the removal of phenol from aqueous solutions. Algae Lessonia nigrescens Bory (A1) and Macrocystis integrifolia Bory (A2) were cross-linked with CaCl2 to enhance their physical and mechanical properties. The natural clays were chemically-exchanged with salts of tetramethyl ammonium (B1), hexadecyltrimethyl ammonium (B2), and bencyltriethyl ammonium (B3) ions to increase their affinity towards organic substrates. The effects of pH and adsorbent dose were evaluated. pH exhibited a strong effect mainly on the phenol aqueous chemistry. Sorption isotherm results were modelled on the Langmuir and Freundlich equations and complemented with EDX analysis, indicating that adsorption of phenol from water was mostly driven by hydrophobic forces, with the exchanged bentonites being the adsorbents that reported the maximum adsorption capacities. Conversely, a polar surface adsorption is suggested for algae mostly by means of hydrogen bonding formation. These results provide further insight into the adsorption mechanism of phenol and analogues and their use as powerful and cheap adsorbent for the treatment of phenol-containing real wastewater.