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Abstract: The rehabilitation and restoration of land-based ecosystems is a key strategy for recovering the services (goods and resources) ecosystems offer to humankind. The use of nature-based solutions (NBSs) to restore degraded soil functions and improve soil quality can be a sustainable and successful strategy to enhance their ecosystem services by working together with the forces of nature and using well-designed measures that require less maintenance, are more cost-effective, and if constructed in the right way may even be more effective over long periods because nature’s forces can increase the structural efficiency. In this study, we aimed to (i) evaluate the bioremediation capacity of some grasses and their suitability for lawn planting in settlements (in residential and non-residential areas, along roads, etc.) and (ii) propose technological solutions for their practical application in an urban environment. Emphasis was placed on the potential of some perennial grasses and their application for the bioremediation of polluted urban soils, including perennial ryegrass (Lolium perenne L.), crested wheatgrass (Agropyron cristatum L.), tall fescue (Festuca arundinacea Schreb), and bird’s foot trefoil (Lotus corniculatus L.). A case study from the city of Plovdiv (Bulgaria) is presented, together with an effective technological solution for the establishment of urban lawns and the roadside green buffer patches.