Hollow-fiber-based adsorbers for gas separation by pressure-swing adsorption (PSA) was studied experimentally. The high efficiency of hollow-fiber-based adsorbers for gas separation was illustrated by hydrogen separation using fine-powder-activated carbon and molecular sieve as adsorbents. The adsorption equilibrium and dynamics of the hollow-fiber adsorbers were determined. The pressure drop of the gas flowing through the adsorbers was also examined. The adsorbers were tested for hydrogen separation from nitrogen, carbon dioxide, and a multicomponent gas mixture simulating ammonia synthesis purge gas. The PSA systems using the hollow-fiber adsorbers were very effective for hydrogen purification. The high separation efficiency is derived from the fast mass-transfer rate and low pressure drop, two key features of hollow-fiber-based adsorbers.