Macroscopic assembly can create advanced materials with hierarchical structure and translate the properties of individual building blocks into ensembles for specific applications. Here, we demonstrate the fabrication of freestanding graphene oxide (GO) films composed of only two Langmuir-Blodgett-induced monolayers under the synergy of wrinkled GO nanosheets and strong noncovalent interaction between GO and melamine. We found that the strongest noncovalent interaction ever measured (∼1 nN) was a synergistic effect of a charge-transfer interaction and hydrogen bonding. The as-obtained film delivered a large optical transmittance of 84.6% at 550 nm and a high mechanical strength of 45 MPa at a notable elongation of 3.5%. The reduced GO film, with a resistance of 420 Ω sq⁻¹, exhibited excellent electromechanical stability for 10,000 cycles at a bend radius of 1.5 mm. With the merits of a unique structure and outstanding properties, such an ultrathin film demonstrates its potential in the application of all-solid-state flexible supercapacitors.

宏观装配可以创建具有分层结构的高级材料，并将各个构件的属性转换为适合特定应用的装配。在这里，我们展示了在起皱的GO纳米片和GO与三聚氰胺之间强烈的非共价相互作用的协同作用下，仅由两个Langmuir-Blodgett诱导的单层组成的独立式氧化石墨烯（GO）膜的制造。我们发现有史以来最强的非共价相互作用（〜1 nN）是电荷转移相互作用和氢键的协同效应。如此获得的膜在550nm处具有84.6％的大的光学透射率和在3.5％的显着伸长率下的45MPa的高机械强度。还原的GO膜，电阻为420Ωsq ^-1，在1.5 mm的弯曲半径下，表现出出色的机电稳定性，可进行10,000次循环。凭借其独特的结构和出色的性能，这种超薄薄膜证明了其在全固态柔性超级电容器中的应用潜力。