In summary, we synthesized and characterized two solvent-free
neutral 2D coordination polymers. They are rare examples
exhibiting reversible one-step high-temperature SCO behaviors.
The spin transition temperatures are 419 and 416 K for 1 and
2, respectively. Moreover, their unusual thermal stabilities are
confirmed by TG and VT-PXRD analyses. Their frameworks
can be stable up to ∼714 and 690 K for 1 and 2, respectively,
which promise potential applications in extreme conditions.