National infrastructure systems (energy, transport, digital communications, water, and waste) provide essential services to society. Although for the most part these systems developed in a piecemeal way, they are now an integrated and highly interdependent “system of systems.” However, understanding the long-term performance trajectory of national infrastructure has proved to be very difficult because of the complexity of these systems (in physical and institutional terms) and because there is little tradition of thinking cross-sectorally about infrastructure system performance. Here, a methodology is proposed for analyzing national multisectoral infrastructure systems performance in the context of uncertain futures, incorporating interdependencies in demand across sectors. Three contrasting strategies are considered for infrastructure provision (capacity intensive, capacity constrained, and decentralized) and multiattribute performance metrics are analyzed in the context of low, medium, and high demographic and economic growth scenarios. The approach is illustrated using Great Britain and provides the basis for the development and testing of long-term strategies for national infrastructure provision. It is especially applicable to mature industrial economics with a large stock of existing infrastructure and challenges of future infrastructure provision.