Flexible membranes (i.e., paper, cloth, and polydimethylsiloxane (PDMS)) have received extensive attention. The rapid development of flexible microfluidics and electronics and their integration calls for complex substrate structures to allow for multiple functions. Inspired by nature, meta-structured membranes (MSMs) as substrates for fabricating integrated microfluidics and electronics are presented. These flexible and freestanding MSMs are generated by the self-assembly of elastic plastic copolymer nanoparticle photonic crystals on micropatterned PDMS templates. The final MSMs constitute with integrated ordered micro-and nanostructures and exhibit spontaneous liquid transfer, fluorescence enhancement, and intimate skin contact. MSMs with designed patterns can be fabricated by assembling polymer nanoparticles on patterned molds; complicated and highly integrated electro-microfluidics are generated on one slice of MSMs by utilizing these patterns as microfluidic channels and electrocircuits. They can be used as chip-on-skin sensors for biochemical-physiological hybrid monitoring sensing of the human body and as organ chips for cell culture and metabolite analysis under drug treatment. Their excellent properties show their potential value in cross-scale sensing and have broad potential applications.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201906745. response and initiative manipulation on one single membrane substrate, which demands interdisciplinary integration. In fact, the combination of microfluidics and electronics on a single membrane has shown great potential in fabricating flexible smart devices such as wearable sensors (skin chips) and organ chips.Considerable attention and efforts have been devoted to fabricating membranes with functions such as super adherence, [4] vivid colors, [5] self-healing, [6] energy harvesting [7] based on micro/ nanostructures. However, the monotonous structure of current membranes limits their performance in flexible smart sensing devices. The construction of robust, ordered-structure membranes as flexible substrates with multiple excellent functions is still anticipated.Among many strategies improving the functionality of membranes, metamaterials or metastructures have widespread concerns. In the past decade, there have been increasing interests in metamaterials (structures) in scientific communities. [8] With the rapid development of materials science and physics, metamaterials are interdisciplinary subjects, including electronic engineering, condensed matter physics, microwave, optoelectronics, classical optics, materials science, semiconductor science, and nanotechnology. [9,10] Among many forms of metamaterials, highly ordered, micro-nano hybrid structures are beyond most striking styles. [11,12] Although there have been some attempts in this field, the high processing cost and complex processing process limit its full application in various fields.Nature provides excellent strategies for the re...