We have studied Ir spin and orbital magnetic moments in the double perovskites La2−xSrxCoIrO6 by x-ray magnetic circular dichroism. In La2CoIrO6, Ir 4+ couples antiferromagnetically to the weak ferromagnetic moment of the canted Co 2+ sublattice and shows an unusually large negative total magnetic moment (-0.38 µB/f.u.) combined with strong spin-orbit interaction. In contrast, in Sr2CoIrO6, Ir 5+ has a paramagnetic moment with almost no orbital contribution. A simple kinetic-energy-driven mechanism including spin-orbit coupling explains why Ir is susceptible to the induction of substantial magnetic moments in the double perovskite structure.

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