Correlated 2D layers, like 1T‐phases of TaS
2, TaSe
2, and NbSe
2, exhibit rich tunability through varying interlayer couplings, which promotes the understanding of electron correlation in the 2D limit. However, the coupling mechanism is, so far, poorly understood and is tentatively ascribed to interactions among the
orbitals of Ta or Nb atoms. Here, it is theoretically...