The increasing number of contaminated sites worldwide calls for sustainable remediation, such as phytoremediation, in which plants are used to decontaminate soils. We hypothesized that better anchoring phytoremediation in plant ecophysiology has the potential to drastically improve its predictability. In this study, we explored how the community composition, diversity and coppicing of willow plantations, influenced phytoremediation services in a four-year field trial. We also evaluated how community-level plant functional traits might be used as predictors of phytoremediation services, which would be a promising avenue for plant selection in phytoremediation. We found no consistent impact of neither willow diversity nor coppicing on phytoremediation services directly. These services were rather explained by willow traits related to resource economics and management strategy along the plant “fast–slow” continuum. We also found greater belowground investments to promote plant bioconcentration and soil decontamination. These traits–services correlations were consistent for several trace elements investigated, suggesting high generalizability among contaminants. Overall, our study provides evidence, even using a short taxonomic (and thus functional) plant gradient, that traits can be used as predictors for phytoremediation efficiency for a broad variety of contaminants. This suggests that a trait-based approach has great potential to develop predictive plant selection strategies in phytoremediation trials, through a better rooting of applied sciences in fundamental plant ecophysiology.