A pilot-scale experimental apparatus was used the mass transfer in a cross-flow rotating packed bed, total volumetric mass-transfer coefficient KLa, effective interfacial area ae were measured by considering the effects of gas velocity, liquid spray density, high gravity factor and gas-liquid contact time with a system of CO2 chemisorption into NaOH solution. The results show that both volumetric mass transfer coefficient and effective interfacial area increase with increasing of gas velocity, liquid spray density and high gravity factor, KLa increases slowly at first and declines sharply with increasing of gas-liquid contact time, while ae decreases slowly with increasing of gas-liquid contact time. The optimal operation conditions are gas velocity 1.69 m/s, liquid spray density 32 m3/(m2×h), high gravity factor 104, and gas-liquid contact time 0.1 s. The mass transfer performance in the present cross-flow rotating packed bed can be enhanced up to 1.52~2.32 times than that reported in the literature under a large gas flow rate. Empirical equations of KLa and ae can be expressed as KLa=1.8221(atDL/dp)ReL0.6371GrL0.0548ScL0.0623 and ae/at=2980.9ReL0.2349FrL-0.045WeL0.5023f-0.5.