Three-dimensional (3D) graphene-based porous materials with a combination of low density, superelasticity, excellent mechanical resilience and tunable functionalities can be used in diverse applications [1-3]. Here we reported a facile approach for the fabrication of macroscopic porous graphene aerogel materials with tunable pore morphology and surface chemistry via a low- temperature and low-cost silane-assisted assembly process [4]. The HI/water solution was utilized to reduce the graphene oxide (GO) in one-step co-assembly process and simultaneously promote the silane bonding reduced GO (silane-b-RGO) under a low temperature of 80 oC and a low GO concentration of 1.0 mg mL-1 in aqueous solution. After the introduction of different types of silane molecule as binder in the 3D RGO aerogels, the pore and wall structures and surface property of the silane-b-RGO aerogels can be controlled/tuned by simply adjusting the type of SCAs and their weight ratio to GO in the initial aqueous solution. The lightweight silane-b-RGO aerogels provides super mechanical performance (90% reversible compressibility), outstanding cyclic resilient property (full recovery after 10 cycles), stable viscoelastic properties and remarkable thermal stability (almost unchanged storage modulus after 100,000 cycles at 300 oC), wide range of density (10-100 mg cm-3), good electrical conductivity (0.1-10 S m-1), excellent hydrophobicity (fast water sliding phenomenon) and extremely high sensitivity of elasticity- dependent conductivity (60-80% at 60% strain). The innovation and improvement in mechanical and other functional properties as well as stabilities lie on the silane chemistry and 3D architecture of the silane-b-RGO aerogels. This opens new opportunities for the preparation of flexible and lightweight graphene aerogel materials with tunable functionalities at both the microstructure and macrostructure, which would benefit technologies such as pressure sensor, high-performance polymer nanocomposite and other filtration/separation applications.