In the present work, four new Ni-II clusters with nuclearities ranging between Ni-4 and Na2Ni8 were synthesized, employing the versatile ligand phenylphosphonate and 6-methylpyridylaldonmate as the coligand. Crystallographic data show that the. tetranuclear complex [Ni-4(6-MepaoH)(4)(PhPO3)(2)(OH)(2)(MeOH)(4)](OH)(2) (1) consists of two dimers linked by phosphonate bridges, whereas [Cs2Ni6(6-Mepao)(6)(PhPO3)(3)(OH)(2)(H2O)(8)] (2), Cs[Ni-8(6-MepaoH)(6)(6-MepaO)(6)(PhPO3)(3)](ClO4)(5) (3), and [Ni8Na2(BzO)(6)(6-Mepao)(6)(PhPO3)(3)] (4) are built from. phosphonato-linked {Ni-3(6-Mepao)(3)} metallacycles. The [9-MCNiII(6-Mepao)(-3)] fragments in 2-4 show the unusual coordination of additional. Cs+, Na-4, and/or Ni-II cations. Direct-current magnetic measurements were carried in the 300-2 K range. Analysis of the experimental data revealed a complex response with strong antiferromagnetic interactions mediated by the oximato bridges and weak interactions mediated by the phosphonate ones.