The establishment of a vegetative cover to enhance evapotranspiration and control runoff and drainage was examined as a method for stabilizing a landfill containing coal combustion waste. Suitable plant species and pretreatment techniques in the form of amendments, tilling, and chemical stabilization were evaluated. A randomized plot design consisting of three subsurface treatments (blocks) and five surface amendments (treatments) was implemented. The three blocks included (1) ripping and compost amended, (2) ripping only, and (3) control. Surface treatments included (1) topsoil, (2) fly ash, (3) compost, (4) apatite, and (5) control. Inoculated loblolly (Pinus taeda) and Virginia (Pinus virginiana) pine trees were planted on each plot. After three growing seasons, certain treatments were shown to be favorable for the establishment of vegetation on the basin. Seedlings located on block A developed a rooting system that penetrated into the basin media without significant adverse effects to the plant. However, seedlings on blocks B and C displayed poor rooting conditions and high mortality, regardless of surface treatment. Pore-water samples from lysimeters in block C were characterized by high acidity, Fe, Mn, Al, sulfate, and trace-element concentrations. Water-quality characteristics of the topsoil plots in block A, however, conformed to regulatory protocols. A decrease in soil-moisture content was observed in the rooting zone of plots that were successfully revegetated, which suggests that the trees, in combination with the surface treatments, influenced the water balance by facilitating water loss through transpiration and thereby reducing the likelihood of unwanted surface runoff and/or drainage effluent.