Graphene oxide (GO) is a basic two dimensional (2D) constructing block that can be utilized to develop high-performance supplies for quite a few functions, significantly within the vitality and environmental fields. Presently, the exact meeting of GO nanosheets into macroscopic nanohybrids of superior power and toughness is fascinating, and faces challenges and trade-offs. Herein, we exploited the freshly established polycationitrile technique as a robust molecular crosslinking technique to engineer ultratough and ultrastrong GO/polymer hybrid movies, during which a covalent triazine-based community was constructed in a light situation to strengthen the interface between GO nanosheets. The tensile power and toughness reached 585 ± 25 MPa and 14.93 ± 1.09 MJ m−three, respectively, which, to the perfect of our information, are the present world data in all GO-based hybrid movies. As an added benefit of the tailored polymer crosslinker, the excessive mechanical efficiency could be maintained largely at an especially excessive relative humidity of 98%. This rising interface-engineering strategy paves a brand new avenue to supply built-in strong-and-tough 2D nanohybrid supplies which are helpful in aerospace, synthetic muscle, vitality harvesting, tissue engineering and extra.