Adsorption is a method widely used to remove low-molecular-weight organics from wastewaters, and phenolic compounds from olive mill wastewater are a persistent class of bioactive pollutants of environmental concern. We screened eleven microalgal candidates at 0.10 g·L⁻¹ using batch kinetics fitted with the Lagergren pseudo-first-order model to obtain rate constants (k) and fitted equilibrium capacities (q_e). Cyanobacteria, particularly Anabaena spp. and Limnospira platensis, exhibited the highest adsorptive potential in the screening; wall-less species (e.g., Dunaliella salina, Isochrysis galbana) showed negligible surface adsorption, indicating that the presence and type of cell wall highly influence biosorption. L. platensis was selected for detailed study because of its established industrial cultivation and valorisation potential. Equilibrium experiments with HCl-functionalized L. platensis at four biomass loadings (0.10–1.00 g·L⁻¹; initial phenolic mix 30 mg·L⁻¹) showed that increasing dose reduced equilibrium concentration (C_e) but decreased specific uptake from ≈77 mg·g⁻¹ to ≈18 mg·g⁻¹ while removal rose from ~26% to ~61%. Nonlinear isotherm fitting favoured the Freundlich model (1/n < 1), consistent with heterogeneous, multi-site adsorption. Targeted macromolecular extractions abolished phenol uptake, demonstrating that the intact protein–polysaccharide matrix is essential for binding. L. platensis route delivered higher single-cycle removal (≈61%) compared to the maize-derived activated carbon reference (≈49%) while also incurring a 1.3-fold lower GWP (approximately 3 kg CO₂-eq per treatment) than the activated carbon route (approximately 4 kg CO₂-eq per treatment) in our model. Overall, L. platensis represents a lower-impact alternative for natural phenols remediation, especially when integrated into valorisation pathways that recover algal co-products.