Molecular spin clusters are mesoscopic systems whose structural and physical features can be tailored at the synthetic level. Besides, their quantum behavior is directly accessible in the laboratory and their magnetic properties can be rationalized in terms of microscopic spin models. Thus they represent an ideal playground within solid state systems to test concepts in quantum mechanics. One intriguing challenge is to control entanglement between molecular spins. Here we show how this goal can be pursued by discussing specific examples and referring to recent achievements.