A bifunctional CaO-Zr/Ni (13, 18, and 20.5 wt% NiO) sorbent-catalyst was developed using the wet-mixing/sonication technique and applied for hydrogen production by sorption-enhanced steam methane reforming (SESMR), an intensified process that integrates hydrogen production with CO2 capture. The material was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and N-2 physisorption (BET). CO2 sorption efficiency of the developed materials was evaluated during 25 CO2 sorption/regeneration cycles. The prepared sorbent-catalysts were then applied in the SESMR during 10 reaction cycles. The results showed that the bifunctional sorbent-catalyst with 20.5 wt% NiO loading presented the most suitable activity. The H-2 yield of similar to 91% at the end of the 10th SESMR cycle is considerably higher than equilibrium H-2 yield that could be obtained by traditional steam methane reforming. (C) 2014 Elsevier B.V. All rights reserved.