We report a facile synthetic protocol to prepare mesoporous FeS2 without the aid of hard template as an electrocatalyst for the hydrogen evolution reaction (HER). The mesoporous FeS2 materials with high surface area were successfully prepared by a sol gel method following a sulfurization treatment in an H2S atmosphere. A remarkable HER catalytic performance was achieved with a low overpotential of 96 mV at a current density of 10 mA.cm(-2) and a Tafel slope of per decade under alkaline conditions (pH 13). The theoretical calculations indicate that the excellent catalytic activity of mesoporous FeS2 is attributed to the exposed (210) facets. The mesoporous FeS2 material might be a promising alternative to the Pt-based electrocatalysts for water splitting.