Three porous organic polymers (POPs) containing carborane were successfully synthesized as adsorbents for gas storage applications, particularly for hydrogen storage. The current physisorption-based materials generally suffer from low isosteric heat of adsorption toward hydrogen molecules. To enhance the interaction between the adsorbent hydrogen, we prepared a series of POPs containing highly electron-deficient carborane components. These polymers have narrow pore size distribution with majority of the dimensions falling in the 0.7- to 1.0-nm range. High Brunauer-Emmett-Teller (BET)-specific surface areas up to 1023m2/g were obtained. Hydrogen adsorption capacities at 77, 195, and 298K were measured using a Sievert isotherm apparatus. The initial heat of adsorption for the carborane -containing polymers was calculated to be 810kJ/mol. Copyright (c) 2011 John Wiley & Sons, Ltd.