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Rational design of transition metal catalysts with robust and durable electrocatalytic activity for hydrogen evolution reactions (HER) is extremely important for renewable energy conversion and storage, as well as water splitting. Heteroatom doping has emerged as a feasible strategy for enhancing electrocatalytic activity. Here, cobalt nanoparticles (Co-NPs) were coated with nitrogen-doped carbon nanotubes (NCNTs) prepared via an in situ growth on accordion-like Ti 3 C 2 T x -MXene (Co-NCNT/Ti 3 C 2 T x). Such an intriguing structure showed great features: abundant anchoring sites for NCNT in situ growth, intimate integration of Co-NPs and NCNTs, high-speed electron transfer between 1D NCNTs and 2D Ti 3 C 2 T x -MXenes, and a large number of effective catalytic active sites. This Co-NCNT/Ti 3 C 2 T x hybrid catalyst was demonstrated to possess excellent HER performance with low overpotential (η 10 , 190 mV), small Tafel slope (78.4 mV dec−1), large electrochemically active surface area, and good long-term stability, thus outperforming many reported electrocatalysts. The present strategy provided a facile route for the design of transition metal HER catalysts with NCNT and MXene. [Display omitted] • The 3D Co-NCNT/Ti 3 C 2 T x catalysts are prepared by a bottom-up approach. • The Ti 3 C 2 T x sheets was connected by NCNT, and high surface area was obtained. • The interconnected porous network is feasible to the high-speed charge transfer. • The as-prepared catalysts possesses superior electrocatalytic ability towards HER. [ABSTRACT FROM AUTHOR]