2D-layered metallic molybdenum disulfide i.e. 1T MoS2 possess prominent electronic conductivity and abundant electrochemically active sites. However, tuning its metastable crystal structure for promoting catalytic performance is a big technical challenge. Here, we reveal the role of the intercalated reducible-NH and-NH2 species as structural stabilizers in supporting the lamellar structure of 1T MoS2, and then propose a novel H2O2-cleaning strategy to reduce the amount of reducible-NH and-NH2 species for modulating the crystallinity and layer thickness of 1T MoS(2 & nbsp;)without degrading to 2H MoS2. The resultant pseudo-1T MoS2 exhibits larger specific surface area (up by 1.6 times) and higher electron mobility compared to original 1T MoS2, leading to excellent photo/electrocatalytic HER activity. Impressively, pseudo-1T MoS2 achieves high visible-light-driven photo-catalytic HER rate of 235.0 mmol.h(-1).g(-1) in combination with CdS. This work offers an extendable crystal structural fine-tuning approach to promote the catalytic activity of metallic transition metal dichalcogenides.