• MIL-101(Cr)-Tu achieved ultrahigh adsorption capacities of 1230.83 mg·g−1 for Au(III), 330.41 mg·g−1 for Pd(II), and 315.58 mg·g−1 for Pt(IV) at 298 K.
• Adsorption kinetics and isotherms follow the pseudo-second-order and Langmuir models, confirming monolayer chemisorption.
• Coordination and electrostatic attraction drive noble metal uptake, with soft–soft interactions between thiourea groups and metal ions; Au(III) and Pt(IV) undergo reduction, while Pd(II) does not.
• The adsorbent shows strong selectivity and excellent reusability, making it a promising candidate for recovering noble metals from secondary resources.