An amphiphilic iron(II) complex [(FeL2)-L-II(NCS)(2), where L is a sub
stituted bipyridine] exhibiting a thermal spin-crossover phenomenon ar
ound room temperature is chemically unstable at the gas-water interfac
e. However, it forms a perfectly stable Langmuir film when formamide-w
ater mixtures are used as a subphase. After transfer onto a solid subs
trate, a well-defined Langmuir-Blodgett (LB) film was then obtained. I
nfrared spectroscopy at variable temperature showed that the spin conv
ersion still occurs in this lamellar material. The specific organizati
on imposed by the LB technique leads to a surroundings effect demonstr
ated, in particular, by thermal cycles. The understanding of this effe
ct is crucial to central any thermal or light-induced spin conversion
within an LB film.