Rational structure design and component-controlled synthesis are attractive and challenging methods to develop materials with unique function for renewable energy conversion such as hydrogen production via water splitting. The earth-abundant and affordable transition metals have been regarded as ideal alternatives to precious platinum. Herein, we report the designed synthesis of component-modified cobalt telluride nanoparticles encapsulated in the nitrogen-doped carbon frameworks with the feature of high surface area and great electron conductivity. Compared with CoTe2/C and CoTe/C, the Co1.11Te2/C presents the highest catalytic activity for HER in 1M KOH due to its structural and component advantages. After a continuous reaction for 20 h or cycling for 1000 cycles, Co1.11Te2/C shows only a little performance loss. This work provides an effective approach to synthesize low-cost and efficient electrocatalysts for HER via rational structural and component design.