The present study investigated the use of algae biorefinery waste and wastepaper in the preparation of cost-effective and eco-friendly xerogels for the removal of congo red (CR) and Fe. The xerogel properties such as density, swelling degree and porosity were modified by incorporating alginate extracted from the brown seaweed Cystoseira trinodis. The developed biosorbents exhibited a light and porous network structure and were characterized by a fast uptake of CR and Fe and adsorption efficiency was increased at pH 6-8. The equilibrium adsorption capacity was found to be 6.20-7.28 mg CR g biosorbent and 8.08-8.39 mg Fe g biosorbent using different xerogels. The adsorption of CR obeyed first-order kinetics, while, Fe followed second-order kinetics. Intraparticle diffusion model suggested a boundary layer effect. The adsorption capacity was maximally obtained as 41.15 mg g and 169.49 mg g for CR and Fe using wastepaper/Spirulina and wastepaper/alginate/Spirulina xerogel, respectively. Temkin isotherm fitted better to the equilibrium data of CR adsorption than Langmuir and Freundlich models. While, equilibrium data of Fe exhibited a best fit to both Langmuir and Freundlich models. Additionally, the Dubinin-Radushkevich isotherm suggested that adsorption mechanism of CR or Fe is predominately physisorption. Investigation of thermodynamic parameters such as ΔH° and ΔS° and ΔG° confirmed the feasibility, spontaneity, randomness and endothermic nature of the adsorption process. Electrostatic attraction, H-bonding and n-π interactions were mainly involved in the biosorption process of CR. The results of this study showed that the developed xerogels could be effectively applied for dye and heavy metal removal at low concentrations.