By auxiliary N-donor ligand-directed assembled, two entangled Co(II)-coordination nets have been constructed from 3,3',5,5'-azobenzenetetracarboxylic acid (H(4)abtc), which present a rare 2D→3D polythreading motif constructed from 2-fold (6,3) polymeric layers with thickness being 10.2 Å and a 3-fold interpenetrating pillar-layered framework based on linear trinuclear Co(II)-SBUs. In addition, two Co(II)-complexes both show an antiferromagnetic coupling by long organic spacers and H(2)O bridges, respectively.