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Motivated by the strategic value of middle-heavy rare earth elements (MHREEs), we proposed a bio-adsorption method to recover ultra-low concentration terbium (Tb(Ⅲ)) from industrial wastewater that originated from the Nd-Fe-B scraps recovery process. It could be found that Tb(Ⅲ) ions as low as 5.34 ng·mL−1(ppb) could be adsorbed onto Ca(Ⅱ)-modified garlic peels (Ca-GP) within 10 min with the adsorption efficiency of 99.2% at pH 3.5. The adsorption behavior of Tb(Ⅲ) onto Ca-GP conformed the Langmuir isotherm model and pseudo-second-order kinetic model. ATR-FTIR, XPS and density-functional theory (DFT) calculations results showed that Tb(Ⅲ) ions could be ion-exchanged with cations in Ca-GP such as Ca(Ⅱ) and -COOH. In application, column experiment results showed that the maximum bed adsorption capacity for Tb, praseodymium (Pr), neodymium (Nd), dysprosium (Dy), and Total rare earth elements (REEs) ions calculated by the Thomas model was 0.06, 3.50, 9.65, 7.34, and 27.37 μg·g−1, respectively, with the initial concentration of 0.37 ng·mL−1 Tb, 20 ng·mL−1 Pr, 44 ng·mL−1 Nd, 67 ng·mL−1 Dy and 170 ng·mL−1 total REEs ions of actual solutions (below the solubility of rare-earth hydroxide). This manuscript thus provided a novel cost-effective and efficient approach to the enrichment and recovery of MHREEs from ultra-low concentration REEs ions-containing solutions. [Display omitted] • Ca(Ⅱ)-modified garlic peels (Ca-GP) biosorbent. • Adsorption of ultra-low concentration of Tb(Ⅲ) (in ppb level) onto Ca-GP. • Ion-exchange of Tb (III) with Ca(Ⅱ) and -COOH of Ca-GP. • Recovery of ppb-level Middle-heavy rare earth from actual solutions. [ABSTRACT FROM AUTHOR]