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‘Cu2(bet)4Cl2’Cl2·4H2O (bet = betaine: IUPAC name: trimethylammonioacetate) is monoclinic, space group P21/c, a = 11.0510(10) Å, b = 14.7140(4) Å, c = 11.1620(15) Å, β = 107.40(2)°. The dinuclear copper(II) cation ‘Cu2(bet)4Cl2’2+ is counterbalanced by two naked Cl− ions. The copper(II) ions have a square bipyramidal environment with oxygen atoms from the acetato groups in the basal planes and a chlorine and a copper atom occupying the apical positions. The metal atoms are μ2-bridged by four acetato groups and the molecular symmetry is close to C2h. The two symmetry-independent chelating betaine molecules are present in their zwitterionic, neutral form.