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Sodium montmorillonite was functionalised by isophorone diisocyanate (IPDI) and organic montmorillonite was functionalised by hydrogenated diphenylmethane diisocyanate (HMDI). Reaction between montmorillonite (MMT) and IPDI/HMDI caused the interlayer space of MMT to increase from 1.41 nm to 1.95 nm and 2.08 nm to 2.42 nm, respectively, and the resulting grafted –NCO groups led to a suitable reactive modifier. In order to improve the high-temperature performance and UV aging resistance of the asphalt binder, asphalt modification was carried out by chemical reaction between –NCO groups and some polar groups (mainly –OH) of asphalt. The results showed that the interlayer space enlarged and exfoliated structure was formed due to the introduction of functionalised MMT (IPDI-HMMT-85 or HMDI-OMMT-80) into the asphalt. The as-prepared IPDI-HMMT-85 and HMDI-OMMT-80 modified asphalts, with a maximum softening point of 57.0 °C and 62.2 °C, initial decomposition temperature of 363 °C and 374 °C, respectively, possessed good storage stability, and were superior to Na-MMT modified asphalt and OMMT modified asphalt in terms of high temperature and UV aging properties.