Tailoring molybdenum selenide electrocatalysts with tunable phase and morphology is of great importance for advancement of hydrogen evolution reaction (HER). In this work, phase‐ and morphology‐modulated N‐doped MoSe2/TiC‐C shell/core arrays through a facile hydrothermal and postannealing treatment strategy are reported. Highly conductive TiC‐C nanorod arrays serve as the backbone for MoSe2 nanosheets to form high‐quality MoSe2/TiC‐C shell/core arrays. Impressively, continuous phase modulation of MoSe2 is realized on the MoSe2/TiC‐C arrays. Except for the pure 1T‐MoSe2 and 2H‐MoSe2, mixed (1T‐2H)‐MoSe2 nanosheets are achieved in the N‐MoSe2 by N doping and demonstrated by spherical aberration electron microscope. Plausible mechanism of phase transformation and different doping sites of N atom are proposed via theoretical calculation. The much smaller energy barrier, longer HSe bond length, and diminished bandgap endow N‐MoSe2/TiC‐C arrays with substantially superior HER performance compared to 1T and 2H phase counterparts. Impressively, the designed N‐MoSe2/TiC‐C arrays exhibit a low overpotential of 137 mV at a large current density of 100 mA cm−2, and a small Tafel slope of 32 mV dec−1. Our results pave the way to unravel the enhancement mechanism of HER on 2D transition metal dichalcogenides by N doping.