Entanglement is an intriguing property of quantum systems that is essential for the implementation of quantum information processing. We review recent results on the establishment of magnetic coupling and spin entanglement between molecular clusters of Cr 7 Ni antiferromagnetic rings. We firstly present the magnetic features of the molecular building blocks and the strategy to link them without altering their properties. A systematic study of the magnetic interaction in (Cr 7 Ni) 2 dimers through different heteroaromatic linkers is then reported. Finally, for the dimer with strongest coupling, the entanglement is directly investigated both theoretically and experimentally.