We show how fibre/matrix interface (or interphase) modification can be used to develop a range of novel carbon fibre reinforced polymer (CFRP) composites that open up new applications far beyond those of standard CFRPs. For example, composites that undergo pseudo-ductile failure have been created through laser treatment of carbon fibres. Composites manufactured with thermo-responsive interphases can undergo significant reductions in stiffness at elevated temperatures. Additionally, structural supercapacitors have been developed through a process that involves encapsulating carbon fibres in carbon aerogel.