With rapid urbanization, the generation of municipal solid waste is growing, placing ever-increasing pressure on cities to close, remediate and repurpose landfill sites in environmentally sustainable and climate-adaptive ways. Traditional landfill final covers such as compacted clay and geosynthetic systems are intended to limit infiltration; yet their conceptual designs often fail in performance longevity due to effects such as desiccation, settlement, root intrusion, freeze–thaw cycling and extreme rainfall. Phytocapping, or evapotranspiration/store-and-release cover technology is the use of vegetated soil profiles to provide storage for percolating rainfall, return water to the atmosphere through evapotranspiration and support biologically mediated oxidation of methane. Phytocapping is a green-inclusive nature-based climate adaptation strategy for urban landfill closure. This study explores hydrological performance, methane mitigation, ecological co-benefits, economic feasibility, climate sensitivity, monitoring requirements and regulatory barriers linked to phytocapping systems. Field evidence is strongest in Australia and the United States, especially through ACAP- and A-ACAP-style programs, while evidence from humid tropical, monsoon, freeze–thaw and low-resource urban contexts is comparatively lacking. As reported in published studies, well-designed phytocaps can result in reduced percolation compared to traditional clay caps. Reported publications also mention considerable construction-cost savings, depending on site conditions and design assumptions. Methane-related outcomes vary by measurement method and site context, with studies reporting surface flux reductions, methane oxidation and landfill gas attenuation as distinct performance indicators. These advantages are counter-balanced by design uncertainties that vary from site to site, limited long-term monitoring data, climate transferability concerns, and regulatory systems still firmly anchored in prescriptive low-permeability barriers. This review proposes a policy-oriented analytical framework that bridges the gap between technical performance evidence, urban co-benefits, staged monitoring and performance-based landfill closure regulation. As such, phytocapping should be considered not as a general-purpose substitute for engineered covers, but as a climate-responsive nature-based solution that can complement urban waste servicing infrastructure, ecological restoration and adaptive governance of landfills when properly designed, monitored and regulated.