Interfaces between different materials, for instance, electrode-dielectrics and vacuum/ air/SF 6 -insulators and oilpaper, are universal in high-voltage insulation systems. Targeted tailoring of the interfacial properties, e.g. chemical structures, micro-/nanoscale morphology, the charge injection barrier, trap states, and surface conductivity, is thought to be an effective approach to improve insulation properties such as breakdown and flashover strength, corona/tracking resistance, and wettability. In this article, the authors review recent progress in interface tailoring methods and their application to improve various insulation properties. The potential application scenarios of interface tailoring in different facilities are first summarised, and the desired insulation properties of various applications are highlighted. Interface tailoring methods are classified as physical/ chemical surface modification and surface coating (inorganic, organic and composite), and the features of different techniques are described in detail. The structure-property relationships between interfacial states and various microscopic parameters such as charge injection barrier, trap distribution and surface conductivity are discussed together with the tailoring mechanisms for different insulation properties. Finally, the future development prospects of interface tailoring methods and their applications, e.g. multifunctional coating and stimuli-response smart coating, are presented.This is an open access article under the terms of the Creative Commons Attribution-NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.