The dinucleating macrocycles H,(Lm") containing two 2,6-di(aminomethyl)-4-methylphenol entities combined through two alkane chains, -(CH,),-(m=2, 3) and -(CH,),-(n=2, 3, 4, S), at the amine nitrogens, form mckeI(I1) complexes of the general formula [Nr2(Lmn)(OA~)2] ((m,n)=(2,2), (2,4), (2,5), (3,3)) and [Nr,(L'*')(OAc)(NCS)(CH,OH)]. [Ni,(L',')(OAc),] . 10HzO crystalhzes m the triclinic system of space group Pl with a = 9.983(2), b = 12.832(2), c = 7.932(l) A, LY= 101.29(l), /I= 101.08(2), y= 106.57(2)", V=921.1(3) A' and Z= 1. The refinement converges with R=5.65 and R,=5.89% based on 2308 reflections with IF,] >3u(lF,]). The macrocycle adopts a folded conformation and each nickel has a cis-p octahedral geometry with the N202 donor set of the macrocycle and two oxygens of a bidentate acetate group. The Ni-Ni separation bridged by two phenolic oxygens IS 3.004 A and the Ni-0-Ni angle is 95.6". Cryomagnetic properties (4.2-300 K) of the complexes are well reproduced based on the spin Hamiltonian Z = -XS, .S2 -D(.S,,'-S,,') with a positive exchange integral (J= + 10.1 to + 2.1 cm-') and a negative zero-field splitting parameter (D= -0.53 to -2.40 cm-'). Each complex shows two reduction waves and two oxidation waves attributable to the metal centers.