Reverse osmosis is widely used as one of the most effective and advanced technologies for the treatment of leachate from landfill sites. Unfortunately, high leachate contamination—above all, ammonia nitrogen—affects membrane selectivity and is reflected in permeate quality. Furthermore, iron contained in leachate can facilitate chelates forming, which reduces the membrane anti-fouling capacity. The addition of a pre-treatment step could alleviate the adverse impact of the pollutants. As such, we investigated pollutant removal by phycoremediation. Initial ecotoxicity tests of three algal strains (Scenedesmus obliquus (S. obliquus), Desmodesmus subspicatus (D. subspicatus), and Chlorella vulgaris (C. vulgaris)) identified D. subspicatus as the strain most tolerant to leachate toxicity. Subsequently, D. subspicatus was cultivated in six landfill leachates of different origin and, after the cultivation, removal rates were determined for ammonia nitrogen and iron. Furthermore, the impact of input leachate parameters on remediation efficiency was also investigated. By phycoremediation, the reduction of up to 100% in iron and 83% in ammonia nitrogen load was achieved, which demonstrates the high potential of microalgae to mitigate environmental risks and reduce membrane foulant content.