Two-dimensional
(2D) metal–molecule hybrid frameworks have
attracted great attention due to their π–d interactions
for the charge–spin–lattice coupling, promising for
next-generation molecular electronics. However, a high electrical
conductivity is indispensable to realize such potential. Herein, we
design and assemble a conductive 2D conjugated coordination thin film
through an interfacial reaction between the aqueous and organic phases.
Its electronic conducting properties are derived from the π–d
coupling interactions to achieve an electrical conductivity of 1.05
S/cm, while the stimulus-dependent π–d interactions induce
multifunctional sensory capabilities. The Co–DABDT (DABDT =
2,5-diamino-1,4-benzenedithiol dihydrochloride) thin films demonstrate
an excellent performance for sensing light, strain, temperature, and
humidity, as well as robust mechanical stability. The 2D frameworks
with multisensing properties for real-time static and dynamic monitoring
are promising for smart wearable electronic systems.