The temperature-induced spin crossover of iron(II) in the [Fe(tpa)(NCS)2] complex has been investigated by nuclear forward scattering (NFS), nuclear inelastic scattering (NIS), extended X-ray absorption fine structure (EXAFS) spectroscopy, conventional Mössbauer spectroscopy (MS) and by measurements of the magnetic susceptibility (SQUID). The various measurements consistently show that the transition is complete and abrupt and exhibits a hysteresis between 102 and 110 K. The dependence of the hyperfine parameters of the high-spin (HS) and of the low-spin (LS) phase on temperature is gradual while the effective thickness (determined by the Lamb-Mössbauer factor fLM) shows a step at the transition temperature. This step could be identified clearly because the effective thickness is measured directly by NFS. The Lamb-Mössbauer factor, the Debye temperature and the mean-square displacement of iron(II) could be determined for the HS and for the LS phase. When comparing the NIS data with the results from density functional theory (DFT), the Fe-N stretching vibrations of both LS and HS phases could be unambiguously identified and the fLM could be factorized for both phases into a lattice and a molecular part. The structural information from EXAFS and DFT geometry optimization are in reasonable agreement.