Electrical conductivity modulation coupled to a high-spin-low-spin conversion in the molecular system [FeIII(qsal)2][Ni(dmit)2]3.CH3CN.H2O.

The synergy between the electrical conductivity within the stacks of Ni(dmit)2 in the newly electrocrystallized [Fe(qsal)2][Ni(dmit)2]3.CH3CN.H2O and the spin conversion of Fe(qsal)2 is evidenced. In addition, the presence of a light-induced excited spin state trapping effect suggests that this complex is a prototypal photoswitchable spin-crossover molecular conductor.