▎ 摘　　要

Macroscopic graphene paper is fabricated by an electrospray deposition approach, and the microstructure can be controlled from highly porous to highly compact geometries by varying deposition parameters including graphene colloid concentration and deposition rate. Free-standing graphene films can be separated from substrates via a simple water exfoliation method in which the surface properties of graphene films and substrates control film exfoliation. Specifically, water exfoliation can be achieved when the contact angle of substrates is 64 degrees or below. Thermal and electrical conductivities of the macroscopic graphene paper upon thermal annealing are measured, enabling the establishment of the process-microstructure-property correlation beneficial for further development and property manipulation of graphene-based materials. Published by AIP Publishing.