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A two‐step sol–gel method is adopted to prepare an iron–calcium hybrid absorbent (Ca–Al–Fe) integrating iron catalysis component and inert support with CaO for calcium looping gasification. Effects of Ca–Al–Fe on cyclic CO2 capture reactivity, mechanical strength, and enhanced reforming of biomass tar model component (toluene) are investigated by comparing with three reference absorbents. Results show that main components of Ca–Al–Fe are CaO, mayenite (Ca12Al14O33), and brownmillerite (Ca2Fe2O5). Ca12Al14O33 plays key roles in keeping stable cyclic carbonation reactivity and significantly promotes mechanical strength of the novel absorbent. In comparison with other absorbents without coupling Ca12Al14O33 or Ca2Fe2O5, Ca–Al–Fe approaches the highest toluene conversion (around 60%) and has the lowest coke deposition (12.2 mg g−1), due to the synergetic influences of Ca2Fe2O5 and Ca12Al14O33, which significantly promotes hydrogen production while reducing CO2 yield in reforming syngas. In addition, influences of reaction conditions such as iron loading, reaction temperature, molar ratio of H2O to carbon in toluene, and absorbent particle size on toluene reforming are examined in the presence of Ca–Al–Fe. Potential reaction routes of toluene reforming are also analyzed and discussed. [ABSTRACT FROM AUTHOR]