The synthesis of iridium oxide decorated erbium pyrosilicate (Er2Si2O7:IrO2) was performed by a simple sol-gel technique. By simple alteration of the reaction parameters, different shapes (i.e., cubes, rods, large spheres, small spheres, and sheets) of Er2Si2O7:IrO2 were obtained and their catalytic activities were tested toward the hydrogen evolution reaction (HER). Among the different morphologies of Er2Si2O7:IrO2, cube-shaped nanoparticles (Er2Si2O7:IrO2-5) with sharp edges provided promising HER activity over a wide pH range from 0 to 14 in acidic, neutral, and basic media. Er2Si2O7:IrO2-5 exhibited an onset potential of -0.076 V with a very high current density of 252 mA cm(-2) (at -0.54 V). The overpotential and Tafel slope for the HER using Er2Si2O7:IrO2-5 were found to be 130 mV and 49 mV/dec, 170 mV and 59 mV/dec, and 190 mV and 67 mV/dec in 0.5 M H2SO4, 1.0 M KOH, and 2.0 M PBS, respectively. The low cost, highly active electrocatalyst shows robust durability over acidic medium for nearly 250 min. Such a superior catalytic activity can be attributed to the synergistic effect between IrO2 and erbium pyrosilicate, in which the 4f orbital (not fully occupied) of rare-earth elements may have occupied the 5d orbital and become valence electrons, resulting in the improved HER activity.