vapor deposition method [3] or on graphene oxide sheets [4] and exert influence on the performances of 3D graphene architectures (TDGAs) in their own way. It has been reported that deformations change local strain distributions, cause curvatures which may induce π-cloud re-hybridization, and modify the electronic structure, local charge distribution, dipole moment and optical properties of graphene. [5][6][7][8] They also alter the local chemical potential due to the formation of electron-hole puddles, [9] tribology properties, [3] thermal conductivity, [10] and mass-transfer behavior. [9] Surface corrugation on the graphene sheets has been confirmed an ideal morphology to be employed in supercapacitors and field emission transistor and give rise to the performances of devices. [11][12][13] Wrinkled graphene has also been proved efficient for applications such as artificial muscles, sensors, vanadium flow battery, laser devices, materials for oil-water separation or with negative Poisson's ratios and so on. [14][15][16][17][18][19] Although there have been lots of reports on graphene-based electrode materials for Li ion batteries, [4,[20][21][22][23] few researches have focused on graphene wrinkling in the context of performances such as mass transport properties and electronics. [24] Consequently, the effects of wrinkles and crumples on performances are not adequately evaluated and elucidated, partly because of multiscale and polybasic application demands. For example, It's reported that the high specific surface area (SSA) of graphene can only be affected by wrinkles up to 2%, regardless of loading conditions, geometry and defects as found by molecular dynamics and continuum mechanics-based simulations in single-layer graphene, but the SSAs of TDGAs may vary in a wide range and are usually far lower than the theoretical SSA of graphene. [3] This means that the conclusions drawn from single-or few-layer graphene adopted in many researches of wrinkles on the properties and structures of materials may be contradict with that of TDGAs. Thus, the influences of graphene wrinkles exposed on performances of TDGAs and TDGAs nanocomposites are of great necessity to be fully evaluated because TGDAs have great potential in applications such as catalysis, sensors, energy storage and conversion. [20,[25][26][27][28] Graphene oxide is a precursor used more widely for construction of TDGAs in view of the numerous oxygen-containing Due to the high in-plane Young's modulus and defects, graphene is prone to deformations such as wrinkles. The effects of wrinkles on the mass and electron transport properties need to be elucidated as graphene has great potential in applications such as catalysis, sensors, energy storage, and conversion. In this paper, the wrinkling of graphene oxide sheets is dominated by the mass ratio of graphene oxide to N,N′-dicyclohexylcarbodiimide (DCC) to fabricate 3D graphene architectures (TDGAs) with tunable porosity. This template-free DCC tactic of regulating the wrinkling procedure forms hierarchical po...