Developing highly efficient noble-metal-free electrocatalysts for hydrogen evolution reaction (HER) has attracted increasing attentions. Here, we report a simple strategy to synthesize the hierarchical "nanoroll" like MoS2/Ti3C2Tx, hybrid by combining liquid nitrogen-freezing and subsequent annealing. The quick freezing of the Ti3C2Tx, nanosheets and ammonium tetrathiomolybdate mixture causes a sudden change in the strain of Ti3C2Tx, which leads to an interesting "nanoroll" like hierarchical structure. After annealing at H-2/Ar atmosphere, vertically aligned molybdenum sulfide (MoS2) crystallites are in situ formed in and on the nanoroll like Ti3C2Tx. Notably, this hierarchical MoS2/Ti3C2Tx hybrid exhibits excellent HER catalytic activity with a small onset overpotential of 30 mV, and a more than 25-fold increase in the exchange current density compared with MoS2 was observed.