The economic and environmental life cycle assessment (LCA) was integrated into a laboratory-based experiment to evaluate the feasibility and sustainability of phytoremediation of chloride-rich marine dredged sediment, using perennial reed Arundo Donax along with biomass valorization. As a prerequisite for life cycle assessments, a baseline mathematical model was developed to estimate the yields of biomass to bioenergy valorization chain including the estimation of biomass yield per m³ sediment, bioenergy yields from valorization schemes, expected green electricity yield, and the phytoremediation time frame. This mathematical model was applied to develop a parametric life cycle inventory for two scenarios of sediment phytoremediation separately or integrated with biomass valorization, for LCA and further sensitivity and uncertainty analysis. Comparative LCA unveiled that the cost and environmental impacts of annual phytoremediation of 1m³ sediment alone or integrated with biomass valorization are much inferior to the corresponding sediment landfill as the inevitable alternative approach for sediment management. With the chloride bioaccumulation capacity of 9940 mg per kg dry biomass of A. donax, the phytoremediation of sediment with chloride concentration higher than 1650 mg/kg may not be achievable in a realistic time frame. Due to the importance of considering sediment depth and the effectiveness of the plant rooting system in estimating the performance of phytoremediation and the time frame, the volume of sediment (1m³) is a more appropriate functional unit than the surface area (ha) for LCA studies of phytoremediation. In addition, considering the volume of sediment as a functional unit retains comparability to other valorization scenarios such as sediment incorporation in cementitious matrices and management scenarios such as landfill, which are generally expressed on a volume or mass basis. Integrating biomass-derived bioenergy production into phytoremediation could offer local and global benefits in terms of economy and environment mainly due to carbon sequestration and avoiding fossil-based fuels.