In view of the encouraging results obtained for the adsorption and release process of hydrogen molecules in Fe(bpac)Fe(CN)4 and Fe(pz)Fe(CN)4, we further investi-gate the feasibility of the proposed spin-crossover strategy for a MOF that has already been synthesised. This is Fe2(tpt)2(NCS)4 (tpt = 2,4,6-tris(4'-pyridyl)-1,3,5-triazine) which was synthesised by C. J. Kepert and coworkers and exhibit Fe(II) in a square-pyramidal coordination. In our calculations, all solvant molecules are removed from the .cif file obtained from the CoRE database. This MOF consists of two interpenetrated structures in which each metal node is coordinated via three tpt ligands. The structure around the open metal center upon gas adsorption is shown in Fig. . The Fe(II) is coordinated with two tpt and two NCS ligands on the xy plane and with another tpt along the z direction. In the absence of host molecules, the ligand field splitting induced by the ligand along z is not strong enough to stabilise the LS state and thus the magnetic fundamental state in the bare MOF is HS. Upon adsorption of H2 on the open metal site, the ground state is LS as a result of the strong binding interacting as expected from a Kubas mechanism. The binding distances between H2 and the Fe are 2.74 A and 1.72 A for HS and LS respectively. These distances and the associated binding geometries are very similar to the those obtained in the case of Fe(bpac)Fe(CN)4 and Fe(pz)Fe(CN)4. The computed ∆EH-L between S=2 and S=0 upon gas adsorption is 0.342 eV. Because of geometrical instability in the LS case of the bare MOF, we could not compute the change in the binding energy associated with the change in the spin state. Nevertheless, the change in the magnetic ground state (it becomes LS) upon H2 adsorption as well as the computed adsorption geometries clearly show that the interaction between the molecule and the MOF is significantly reduced when switching from S=0 to S=2.