The synthesis of two nickel(II) complexes based on a central bridging triaminoguanidine
scaffold and a capping ligand per metal ion is reported. When 2,2′-bipyridine (bipy) is utilized as co-ligand the complex [Ni
3L
Br(bipy)
3(H
2O)
3]NO
3 · 9H
2O · 1.5DMF (
1) is obtained which crystallizes in the hexagonal space group
P63/m. Complex
1 shows an interesting supramolecular structure pattern with alternating hydrophilic and hydrophobic layers characterized by extensive hydrogen-bonding and π–π-stacking, respectively. With 2,4,6-(2-pyridyl)-1,3,5-
triazine (tptz) as capping ligand, complex [Ni
3L
Br(tptz)
3]ClO
4 · 7H
2O · 1.5DMF (
2) is obtained. The magnetic susceptibility data can be fitted using an equilateral triangle model (
![Click to view the MathML source](http://www.sciencedirect.com/cache/MiamiImageURL/B6TG5-4NJ20J1-3-14/0?wchp=dGLzVlz-zSkWz)
) with an isotropic coupling constant of
J=-31.0±0.6 for
1 and
![Click to view the MathML source](http://www.sciencedirect.com/cache/MiamiImageURL/B6TG5-4NJ20J1-3-16/0?wchp=dGLzVlz-zSkWz)
for
2.