Spin-crossover (SCO) complexes featuring hidden spin states have recently garnered significant attention. The hidden states are challenging to access via a routine cooling strategy due to the extremely slow dynamics of the SCO process, however, they are accessible via light irradiation. In this study, we prepared two homochiral mononuclear Fe-II complexes [(S(R)-L)Fe(NCBH3)(2)]center dot MeOH (S1 and R1, S/R-L = (S/R)-N-1,N-2-dibenzyl-N-1,N-2-bis(pyridin-2-ylmethyl)propane-1,2-diamine), as well as their desolvated counterparts, S1d and R1d, which can be interconverted through a single-crystal ...