The separation of hydrogen isotopes remains a significant challenge due to their nearly identical physicochemical properties. Recently, metal-organic frameworks employing the chemical affinity quantum sieving effect have garnered increasing attention for hydrogen isotope separation. In this study, Cu-BTT with open metal sites was synthesized and demonstrated high hydrogen isotope adsorption capacities of 266 cm3/g for H2 and 288 cm3/g for D2. Dynamic breakthrough experiments revealed a selectivity of 1.58 at 77 K, highlighting the potential of Cu-BTT as a promising candidate for hydrogen isotope separation.