The competing and non‐equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium‐7,7,8,8‐tetracyanoquinodimethane (K‐TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm−2, 10 Hz) in such a molecular electronic crystal initiates a stable long‐lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge–spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high‐pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge–spin–lattice decoupling to activate and subsequently stabilize nonequilibrium phase. The cooperativity triggered by ultrahigh‐strain‐rate (above 106 s−1) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro‐magnetic phases with technological promises.

Electrically switchable magnetic and electronic properties are promising for quantum sensing and information technology. Here, we report an electrically driven magnetic and electronic phase transition in molecular electronic crystal, potassium-7,7,8,8-tetracyanoquinodimethan, with the magneto-electric switching over 105 cycles at room temperature. Electron spin resonance study reveals the cooperative transition between spin and charge degrees of freedom. In addition, the mechanistic spectroscopy studies suggest the charges in an inhomogeneous conductor–insulator mixed state. The findings shown here suggest electrically controlled ordering in strongly correlated molecular crystal leads to dynamic magneto-electric switching, paving the way for developing molecular-based memory and switching devices.

Supramolecular Electronic Crystals The cooperative tuning of a supramolecular electronic crystal enables access to a long‐lived hidden conducting phase with a broad temperature range from 2 to 360 K, through a pulsed electromagnetic field. In article number 2103000, Shenqiang Ren and co‐workers demonstrate a a dynamic and cooperative phase in K‐TCNQ, with the control of pulsed electromagnetic excitation. A dedicated charge–spin–lattice decoupling is required to activate and subsequently stabilize the non‐equilibrium phase.