The crystal phase plays an important role in controlling the properties of an anomaterial;h owever,i ti s ag reat challenge to obtain ananomaterial with high purity of the metastable phase.F or instance,the large-scale synthesis of the metallic phase MoS 2 (1T-MoS 2 )isimportant for enhancing electrocatalytic reaction, but it can only be obtained under harsh conditions.Herein, aspatially confined template method is proposed to synthesizeh igh phase-purity MoS 2 with a1 T content of 83 %. Moreover,b oth the confined space and the structure of template will affect the purity of 1T-MoS 2 ;i nt his case,t his approach was extended to other similar spatially confined templates to obtain the high-purity material. The obtained ultrathin nanosheets exhibit good electrocatalytic activity and excellent stability in the hydrogen evolution reaction.Nanomaterials have shown various promising applications in optics, [1] catalysis, [2] and electronics, [3] owing to their unique physiochemical properties,w hich strongly depend on the crystal facet, morphology,d imension, and size.I nr ecent years,t he crystal phase has been reported as an important factor to affect the physical-chemical properties.F or exam-ple,M oS 2 is at ypical polyphase material which includes trigonal (1T), hexagonal (2H), rhombohedral (3R), and 1T' forms. [4] Among them, the unique structure of 1T phase MoS 2 endows it with am etallic-like property, [5] showing higher electrical conductivity and catalytic activity. [6] Nevertheless, the thermodynamically stable phase for MoS 2 is 2H;h ence, the metastable 1T MoS 2 can only be obtained under the harsh synthetic strategies,s uch as alkali metal intercalation-exfoliation, [7] mechanical strain, [8] and electron-beam irradiation. [6a] However,the yields of the aforementioned methods are quite low,w hich severely limits the applications of metallic-phase MoS 2 . [9] It is agreat challenge to obtain high-purity 1T MoS 2 with af acile method. [8] By using the weak interactions between hetero materials, template method is considered as an efficient route to synthesize nanomaterials with metastable phases. [10] Moreover, the confined space will significantly affect the physical and chemical properties of the insert molecules. [11] In this case,t he two-dimensional confined space may induce a2 D nanosheet with metastable phases.T herefore,b yu sing layered Ni(OH) 2 as the spatially confined template,w e successfully synthesized ultrathin MoS 2 nanosheets with the 1T phase of 83 %, which is among the highest 1T ratios obtained with the wet-chemical methods (Supporting Information, Table S1). Af urther study reveals both the space in the confined template and the crystal structure of template will affect the crystal phase of nanomaterials.M oreover,t he ratio between 1T and 2H phases can be easily controlled by adjusting the structure of templates.F urthermore,t he synthesized nanosheets showed an excellent catalytic activity and stability for the hydrogen evolution reaction (HER). Our strategy provides an ew way to...