The ground-state spin arrangement and the bipartite entanglement within Cu 2+ -Cu 2+ dimers across the magnetization process of the 4f-3d heterometallic coordination polymer [Dy(hfac) 2 (CH 3 OH) 2 Cu(dmg)(Hdmg) 2 ] n (H 2 dmg = dimethylglyoxime, Hhfac = 1,1,1,5,5,5-hexafluoropentane-2,4-dione) are theoretically examined using the symmetric isotropic spin-1/2 Ising-Heisenberg orthogonal-dimer chain. The numerical results point to five possible ground states of the compound with three different degrees of the quantum entanglement within Cu 2+ -Cu 2+ . Besides the standard ferrimagnetic and saturated phases without quantum entanglement of Cu 2+ ions, which are manifested in low-temperature magnetization curve as wide plateaus at the non-saturated magnetization 16.26µ B and at the saturation value 20.82µ B , respectively, one also finds an intriguing singlet-like phase with just partial entanglement within Cu 2+ -Cu 2+ and two singlet phases with fully entangled Cu 2+ -Cu 2+ dimers. The former quantum phase can be identified in the low-temperature magnetization process as very narrow intermediate plateau at the magnetization 9.27µ B per unit cell, while the latter ones as zero magnetization plateau and intermediate plateau at the magnetization 18.54µ B . Non-monotonous temperature variations of the concurrence, through which the entanglement within cooper dimers is quantified, point to the possible temporary thermal activation of the entangled states of Cu 2+ -Cu 2+ also above non-entangled ferrimagnetic and saturated phases.