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The thermal conductivity/diffusivity of pearlitic grey irons with various carbon contents was investigated by the laser flash method. The materials were cast in controlled thermal environments producing three dissimilar cooling rates. The cooling rates together with the carbon content largely influence the thermal conductivity of grey iron. Linear relationships exist between the thermal conductivity and the carbon content, the carbon equivalent, and the fraction of the former primary solidified austenite transformed into pearlite. The results show that the optimal thermal transport properties are obtained at medium cooling rates. Equations are given for the thermal conductivity of pearlite, solidified as pre-eutectic austenite, and the eutectic of grey iron. The thermal conductivity of pearlitic grey iron is modelled at both room temperature and elevated temperatures with good accuracy.