Phytoremediation is an economic way to attenuate soil heavy metal pollution, but is frequently limited by its low pollutant-removing efficiency. Recently, we revealed the close relation between polysaccharide-based biofilm formation and cadmium removal. In this study, for improving the phytoremediation efficiency, an artificial polysaccharide-binding protein was designed by synthetic biology techniques to regulate biofilm formation. The artificial protein Syn contained two polysaccharide-binding domains from the Ruminococcus flavefaciens CttA and the Clostridium cellulolyticum CipC, preferentially binding polysaccharides exposed on both cadmium-treated bacteria and plant roots. Under cadmium stress, Syn remarkably promoted bacterial polysaccharide production from 99 mg/L to 237 mg/L, leading to 1.23-fold higher biofilm biomass. During treatment of the remediation plants with exogenous cadmium-capturing bacteria, Syn improved root biofilm formation, with the root surface polysaccharide contents increasing by 79%, and the Log10 CFU/g root increasing from 7.01 to 7.80. Meanwhile, Syn remodeled the rhizosphere microbiome, especially increasing the abundance of the bacterial groups involved in biofilm formation and stress tolerance, e.g., Pseudomonas, Enterobacter, etc. Consequently, Syn promoted plant cadmium adsorption, with the cadmium-removing efficiency increasing from 17.2% to 33.8%. This study sheds light on synthetic biology-based regulation of biofilm formation for enhanced phytoremediation. Display omitted •Cadmium gently induces biofilm formation of cadmium-capturing bacteria.•The artificial protein Syn exhibits high capacity to bind polysaccharides.•Syn strongly promotes functional biofilm formation on roots of remediation plants.•Syn increases the rhizosphere abundance of biofilm-related bacterial groups.•Syn strongly enhances soil cadmium removal by the remediation plants.