A common problem of many approximate functionals is the erroneous description of charge transfer (CT) states due to unphysical electronic self-interaction. This problem can be alleviated by including exact exchange interaction from Hartree-Fock theory in the functional. While hybrid functionals such as B3LYP do this in a fixed manner, a more balanced inclusion can be realized in range-separated functionals. These functionals include exact exchange weighted with a damping function that depends on the inter-electronic distance, ensuring a smooth transition from the short-to the long-range domain. This approach aims at minimizing the spurious electron's self-interaction energy and mitigating the (de)localization error. It remains then only necessary to determine the steepness of the damping function, a feature that can be obtained for the individual system by tuning the energetic positions of highest-occupied (HOMO) and lowest unoccupied molecular orbitals (LUMO) to fit the ab initio ionization potential (IP) and electron affinity (EA). Despite that tuned range-separated functionals have been shown to be very useful for describing properties related to fundamental and optical energy gaps, it can be non-trivial to obtain a unique set of rangeseparation parameters, particularly if one needs to describe both CT and locally-excited states on the same footing. Furthermore, it is far from obvious whether different parameters would ultimately lead to the same relaxation mechanisms after light irradiation. Thefore, in this work, we critically examine the performance of several range-separation parameters on the absorption spectrum, PESs and ultimately on the excited state dynamics of the Fe(II) complex [Fe(cpmp) 2 ] 2+ (see Fig. ), where cpmp = 6,2"-carboxypyridyl-2,2'-methylamine-pyridyl-pyridine is a push-pull ligand used previously in an analogous ruthenium(II) compound. This complex, recently synthesized and experimentally characterized, follows two strategies for achieving long-sought long-lived MLCT states: forming a close to octahedral coordination of the central iron that maximizes the ligand-field splitting, and destabilizing the MC states by electron-rich ligands while simultaneously stabilizing the MLCT states by π-acceptor groups, such as in other iron(II) push-pull complexes. We first investigate different routes to tune the rangeseparation parameters of the LC-BLYP functional (Section II). Since we obtain different sets of range-separation parameters, we benchmark their accuracy using experimental data and the more accurate multi-reference wave function based method CASPT2 (Section III). We then use the two most promising sets of range-separation parameters to parametrize the PESs, on which TSH molecular dynamics simulations are carried out (Section IV). To our sur-prise, the simulated photodynamics display strikingly different mechanisms that can be traced back to the different electronic characters for some of the states for the two sets of parameters. In order to decide which one is the correct mechanism, we leverage time-resolved spectroscopic experiments, highlighting how in this case theory alone can struggle to provide the correct dynamical picture and how easily one can be lead astray.