discovered metastable phase. It has the highest intrinsic T c of 8.9 K among all the TMDs. [5] Its crystal structure has a symmetry of a monoclinic space group C2/m. The crystal structure of 2M-WS 2 has a different stacking order along the c-axis, compared with the known T d -WTe 2 or 1T′-MoTe 2 , where "2" indicates the number of monolayers in each unit cell and "M" represents the monoclinic lattice. [6] Furthermore, the theoretical calculation indicates that hole and electron pockets coexist at the Fermi surface of 2M-WS 2 and this material owns a possible topological surface state. [6] As a newly discovered superconductor in TMDs, little has been known about the properties of 2M-WS 2 . To understand the superconducting state as well as other electronic states, the phase diagram is very important and helpful. As we know, T c can be fine-tuned by the carrier density of the materials. [6] Traditionally, to modulate the carrier density, researchers need to fabricate a series of electrondoped and/or hole-doped samples. Fortunately, electrochemical gating has been employed as an effective way to dope carriers over a wide range. [7] The detailed tuning by lithium intercalation through the charge density wave and superconductivity phase in 1T-TaS 2 classified the universality of the quantum critical point. [8] Furthermore, electrochemical gating can induce the reversible structure transformation. A tristate phase transformation was realized in SrCoO 3−x by using an electric field to control the insertion and extraction of oxygen and hydrogen ions that were electrolyzed from H 2 O. [9] So, upon applying proper gate voltage (V g ), ions in the dielectric electrolyte can be effectively controlled to accumulate on the surface of material or intercalate into the material, thus tuning its electronic states.In this article, we selected the new metastable phase 2M-WS 2 as a model to systematically modulate the carrier density and explore its transport properties by gate-controlled Li-ion intercalation. Primary 2M-WS 2 is a superconductor with a T c of 8.9 K; when the Li-ion polymer gel was dropped on the sample, flake sample underwent a phase transition from a superconductor to an insulator, which is induced by the Li-ion intercalation. The corresponding carrier density changed from 9.05 × 10 21 to −6.04 × 10 20 cm −3 . Interestingly, the process of phase transition is reversible with the intercalation and deintercalation of lithium ions. In particular, our complete phase diagram for the first time provides fresh insights into the relations between the superconducting state and various other electronic states.2M-WS 2 is a metastable phase among TMDs that was first reported in our previous paper. [5] It owns a layered structure with monoclinic space group C2/m, in which each atomic Electrolyte gating has been employed as an effective way to modulate the electronic properties of transition metal dichalcogenides (TMDs) by carrier doping over a wide range. Here, the carrier density of a new metastable phase of TMD material 2M-WS...