One reason arid and semi-arid environments have been used to store waste is due to low groundwater recharge, presumably limiting the potential for meteoric water to mobilize and transport contaminants into groundwater. The U.S. Department of Energy Office of Legacy Management (LM) is evaluating selected uranium mill tailings disposal cell covers to be managed as evapotranspiration (ET) covers, where vegetation is used to naturally remove water from the cover profile via transpiration, further reducing deep percolation. An important parameter in monitoring the performance of ET covers is soil moisture (SM). If SM is too high, water may drain into tailings material, potentially transporting contaminants into groundwater; if SM is too low, radon flux may increase through the cover. However, monitoring SM via traditional instrumentation is invasive, expensive, and may fail to account for spatial heterogeneity, especially over vegetated disposal cells. Here we investigated the potential for non-invasive SM monitoring using radar remote sensing and other geospatial data to see if this approach could provide a practical, accurate, and spatially comprehensive tool to monitor SM. We used theoretical simulations to analyze the sensitivity of multi-frequency radar backscatter to SM at different depths of a field-scale (3 ha) drainage lysimeter embedded within an in-service LM disposal cell. We then evaluated a shallow and deep form of machine learning (ML) using Google Earth Engine to integrate multi-source observations and estimate the SM profile across six soil layers from depths of 0–2 m. The ML models were trained using in situ SM measurements from 2019 and validated using data from 2014 to 2018 and 2020–2021. Model predictors included backscatter observations from satellite synthetic aperture radar, vegetation, temperature products from optical infrared sensors, and accumulated, gridded rainfall data. The radar simulations confirmed that the lower frequencies (L- and P-band) and smaller incidence angles show better sensitivity to deeper soil layers and an overall larger SM dynamic range relative to the higher frequencies (C- and X-band). The ML models produced accurate SM estimates throughout the soil profile (r values from 0.75 to 0.94; RMSE = 0.003–0.017 cm3/cm3; bias = 0.00 cm3/cm3), with the simpler shallow-learning approach outperforming a selected deep-learning model. The ML models we developed provide an accurate, cost-effective tool for monitoring SM within ET covers that could be applied to other vegetated disposal cell covers, potentially including those with rock-armored covers.