The release of effluents containing cadmium ions into aquatic ecosystems is hazardous to humans and marine organisms. In the current investigation, biosorption of Cd2+ ions from aqueous solutions by freely suspended and immobilized Turbinaria ornata biomasses was studied. Compared to free cells (94.34%), the maximum Cd2+ removal efficiency reached 98.65% for immobilized cells obtained via Box–Behnken design under optimized conditions comprising algal doses of 5.04 g L−1 and 4.96 g L−1, pH values of 5.06 and 6.84, and initial cadmium concentrations of 25.2 mg L−1 and 26.19 mg L−1, respectively. Langmuir, Freundlich, and Temkin isotherm models were suitably applied, providing the best suit of data for free and immobilized cells, but the Dubinin–Radushkevich model only matched the immobilized algal biomass. The maximum biosorption capacity of Cd2+ ions increased with the immobilized cells (29.6 mg g−1) compared to free cells (23.9 mg g−1). The Cd2+ biosorption data obtained for both biomasses followed pseudo-second-order and Elovich kinetic models. In addition, the biosorption process is controlled by film diffusion followed by intra-particle diffusion. Cd2+ biosorption onto the free and immobilized biomasses was spontaneous, feasible, and endothermic in nature, according to the determined thermodynamic parameters. The algal biomass was further examined via SEM/EDX and FTIR before and after Cd2+ biosorption. SEM/EDX analysis revealed Cd2+ ion binding onto the algal surface. Additionally, FTIR analysis confirmed the presence of numerous functional groups (hydroxyl, carboxyl, amine, phosphate, etc.) participating in Cd2+ biosorption. This study verified that immobilized algal biomasses constitute a cost-effective and favorable biosorbent material for heavy metal removal from ecosystems.