Three-dimensional (3D) graphene oxide/MXene (GO/MX) composite aerogels with characters of lightweight, porous structure, and superior elasticity have attracted great attention in electromagnetic shielding, oil–water separation, and chemical catalysis, especially smart electronic sensors. However, due to the lack of adequate interaction force between GO and MX nanosheets, it is challenging to construct a high strengthand long-range ordered GO/MX aerogel, resultingin inferior mechanical properties and poor conductivity. Here, a facile gelation strategy is developed to form long-range ordered GO/MX aerogel by ethylenediamine (EDA) induced self-assembly of MX and GO liquid crystals (LCs). In this system, EDA plays dual roles of inducing ordered self-assembly of GO LCs nanosheets and strengtheninginteraction between GO and MX nanosheets. As a result, the obtained GO/MX aerogel with long-range ordered microstructure presents an outstanding mechanical elasticity of 9.5 kPa and a high conductivity of 0.99 S m−1. Especially, the assembled GO/MX-based sensor has an extremely low detection limit of ~ 0.2% strain, prominent physiological signal capture capability, and excellent durability over 10,000 compression/release cycles. This work paves the way for the potential applications of GO/MX composite aerogel in real-time human motion monitor, artificial skins, and flexible smart devices.