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The forms of boron atoms are many and varied in the structure of transition metal borides (TMBs). The form of boron atoms determines the structure, morphology, and properties of borides. Herein, transition metal monoborides (CrB and WB) with different arrangement of one-dimensional (1D) boron chains were synthesized under high pressures and high temperatures. The 1D boron chains between the interlayers of CrB are parallel to one another, while the 1D boron chains between the interlayers of WB are perpendicular to one another. The morphologies of CrB and WB also show large differences due to the difference in 1D boron chain arrangement. As electrocatalysts for hydrogen evolution reactions (HERs), CrB and WB show good catalysis activity and durability. WB has the smallest overpotential (210 mV) and Tafel slope (90.09 mV dec−1), which is mainly attributed to the intercrossing boron chains improving the electrical properties of WB, as well as the 5d electrons of W being more chemically active. The TOF value of WB is 1.35 s−1, proving that WB has a higher intrinsic catalytic activity during HERs. This work provides a data reference for the development of high-efficiency electrocatalysts. [ABSTRACT FROM AUTHOR]