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MIL-101 is a promising metal-organic frameworks (MOFs) material in adsorption chiller application due to its high adsorption capacity for water and excellent adsorption/desorption cyclic stability. Few layer graphene (FLG) as the thermal conductive additive was added into MIL-101 to improve inferior heat transfer of MIL-101 in the adsorption cooling process. The heat transfer characteristic of MIL-101/FLG adsorber and the adsorption cooling performance of the MIL-101/FLG-water working pair were studied. Results show that thermal conductivity of MIL-101/20%FLG composite is 5.79-6.54 times that of MIL-101. Adding FLG is conducive to the formation of heat transfer channels in MIL-101/FLG adsorber and the rapid removal of adsorption heat. The heating and cooling rate of MIL-101/FLG adsorber is ~2.2 times that of MIL-101 adsorber. Under typical adsorption water chiller conditions, the specific cooling power (SCP) and coefficient of performance (COP) of the MIL-101/FLG-water working pair is 72.2–81.0 W kg−1 and 0.187–0.202, respectively, at desorption temperatures of 70 °C and 90 °C, which is 1.43–1.56 times higher than the MIL-101-water working pair. The excellent structural and adsorption/desorption cyclic stability of MIL-101/FLG composite is verified after 50 consecutive cycles. It can provide a promising adsorbent candidate (MIL-101/FLG composite) in adsorption water chiller process.