Low-temperature assembly of MXene nanosheets into three-dimensional (3D) robust aerogels addresses the crucial stability concern of the nano-build-ing blocks during the fabrication process,which is of key importance for transforming the fascinating properties at the nanoscale into the macroscopic scale for practi-cal applications.Herein,suitable cross-linking agents(amino-propyltriethoxysilane,Mn2+,Fe2+,Zn2+,and Co2+) as interfacial mediators to engineer the interlayer interactions are reported to realize the graphene oxide(GO)-assisted assembly of Ti3C2Tx MXene aerogel at room temperature.This elaborate aerogel construction not only suppresses the oxidation degradation of Ti3C2Tx but also generates porous aerogels with a high Ti3C2Tx content (87 wt％) and robustness,thereby guaranteeing the functional accessibility of Ti3C2Tx nanosheets and operational reliability as integrated functional materials.In combination with a further sulfur modification,the Ti3C2Tx aerogel electrode shows promising electrochemical performances as the freestanding anode for sodium-ion storage.Even at an ultrahigh loading mass of 12.3 mg cm-2,a pronounced areal capacity of 1.26 mAh cm-2 at a current density of 0.1 A g-1 has been achieved,which is of practical significance.This work conceptually suggests a new way to exert the utmost surface functionalities of MXenes in 3D monolithic form and can be an inspiring scaffold to promote the application of MXenes in different areas.