Transition metal oxides (TMO) are promising electrochromic (EC) materials for applications such as smart windows and displays, yet challenge still exists to achieve good flexibility, high coloration efficiency and fast response simultaneously. MXenes (e.g. Ti3C2Tx) and their derived TMOs (e.g. 2D TiO2) are good candidates for high-performance and flexible EC devices because of their 2D nature and the possibility of assembling them into loosely networked structures. Here we demonstrate flexible, fast, and high-coloration-efficiency EC devices based on self-assembled 2D TiO2/Ti3C2Tx heterostructures, with the Ti3C2Tx layer as the transparent electrode, and the 2D TiO2 layer as the EC layer. Benefiting from the well-balanced porosity and connectivity of these assembled nanometer-thick heterostructures, they present fast and efficient ion and electron transport, as well as superior mechanical and electrochemical stability. We further demonstrate large-area flexible devices which could potentially be integrated onto curved and flexible surfaces for future ubiquitous electronics.