Five Schiff base ligands have been utilized to explore metallo-pseudohalide (azide or cyanate) systems. These ligands are the 1:1 condensation products of 3-methoxysalicylaldehyde with ethanolamine (H2L1)/1-(2-aminoethyl)-piperidine (HL2)/ 4-(2-aminoethyl)-morpholine (HL3) or salicylaldehyde with 1-(2-aminoethyl)-piperidine (HL4)/4-(2-aminoethyl)-morpholine (HL5). The derived complexes are as follows: Four heterobridged μ-phenoxo-μ1,1-azide/cyanate dinickel(II) compounds of composition [Ni\(^{\rm II}_{2}\)(HL\(^{1})_{3}(\mu_{1,1}\)-N3)]·3H2O (1), [Ni\(^{\rm II}_{2}\)(L\(^{2})_{2}(\mu _{1,1}\)-N3)(N3)(H2O)]·CH3CH2OH (2), [Ni\(^{\rm II}_{2}\)(L\(^{3})_{2}\) (μ1,1-N3)(CH3CN)(H2O)](ClO4)·H2O·CH3CN (3) and [Ni\(^{\rm II}_{2}\)(HL\(^{1})_{3}(\mu _{1,1}\)-NCO)]·2H2O (4); Two μ1,3-azide bridged tetranickel(II) compounds [{NiII(L\(^{4})(\mu _{1,3}\)-N3)(H2O)}4] (5) and [{NiII(L\(^{5})(\mu _{1,3}\)-N3)(H2O)}4] (6); Two μ1,3-azide/cyanate one-dimensional compounds [CuIIL\(^{5}(\mu _{1,3}\)-NCO)] n ·2nH2O (7) and [CuIIL\(^{5}(\mu _{1,3}\)-N3)] n · 2nH2O (8). Except compound 5 which shows overall antiferromagnetic coupling, other compounds exhibit overall ferromagnetic interaction. Syntheses, crystal structures, magnetic properties, density functional theoretical (DFT) calculations and experimental/theoretical magneto-structural correlations have been carried out which have revealed some interesting observations on composition/topology, magneto-structural correlations and solid state isomerism. The results have been already published. The present report deals with a review of the salient and interesting features of these works. This article reviews some recent studies on metallo-pseudohalide compounds, only pseudohalide bridged or heterobridged µ-phenoxo-µ1,1-azide/cyanate complexes, and focuses on the following features: (i) unprecedented type of structures; (ii) unique bridge distance dependency of exchange integral; (iii) experimental and density functional theoretical magneto-structural correlations; (iv) interesting magnetic, crystallographic and supramolecular isomerisms.