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Ti2Cu, TiCu and TiCu4 were synthesized and their electrocatalytic activities for hydrogen evolution reaction (HER) were investigated. The hydrogen overpotential observed at 10 mA/ cm2 (η10) followed the order Ti2Cu (η10 = −215 mV) > TiCu (η10 = −182 mV) > TiCu4 (η10 = −170 mV). The hydrogen adsorption energy (∆GHad) on Cu site of TiCu4 is exergonic and close to optimal position (i.e. ∆GHad = 0). A synergistic effect was proposed to account for the excellent HER performance of these TiCu binary intermetallics compounds that could replace PGM and achieve Midas touch in the future.