The spontaneous self-organization of coordination compounds has been studied intensively over the last few decades.[1] One area of particular interest is the assembly of multistranded helicates. [2][3][4][5] As most strategies for the synthesis of helicates with high nuclearities make use of long and flexible organic ligands, many linear helicates have been prepared. [3, 5] Because of their unique physical and chemical properties, helicates have been used as components of functional materials and devices. [6, 7] These applications could experience remarkable development if clusters with novel properties were introduced into the helicates.There are few examples of cluster helicates, in which metal clusters define the helical axis.[ [9] The Mössbauer spectrum of 1 at 78 K consists of three quadrupole doublets with relative peak areas of 2:1:2, which correspond to two types of high-spin iron(II) ions (isomer shift (IS) = 1.03 mm s À1 , quadrupole splitting (QS) = 3.34 mm s À1 ; IS = 1.03 mm s À1 , QS = 2.81 mm s À1 ) and one type of low-spin iron(II) ion (IS = 0.46 mm s À1 , QS= 0.26 mm s À1 ), respectively (Figure 1).[10] These Mössbauer data are consistent with the structure determined by X-ray diffraction.