In this work, we demonstrate the principle of mesoscopic construction of silk fibroin (SF) hybrid materials, which endows the materials with new performance. In implementing this strategy, mediating molecules, wool keratin (WK) molecules, were adopted to in-line synthesize Au nanoparticles (WK@AuNPs), which further create the stable linkage of AuNPs with SF nanofibril networks via templated β-crystallization. Fourier transform infrared spectroscopy, X-ray diffraction, and atomic force microscopy demonstrate that the mesoscopic hybrid network structure of the hybrid materials is different from neat SF materials, which gives rise to various new performances, that is, long-stable fluorescence emission. As the fluorescence emission can be characteristically annealed by Cu ions, therefore be adopted as the highly selective ion probes. Moreover, as WK@AuNPs are homogeneously connected to SF nanofibril networks, the carbonization of the materials leads to secondary hybrid materials of carbon-Au, where nano-sized Au particles are well distributed in carbonized mesoscopic conductive carbon networks. Such hybrid materials of carbon-Au can be further fabricated into electrochemical (i.e., dopamine) sensors, which are demonstrated to have excellent sensing performance.@en

This work examines the self-collimation effect of silk materials on fluorescence emission/detection. A macroscopic regulation strategy, coupled with meso-reconstruction and meso-functionalization, is adopted to amplify the fluorescence emission of organic fluorescent dyes (i.e., Rhodamine 6G (R6G)) using silk photonic crystal (PC) films. The fluorescence emission can be linearly enhanced or inhibited by a PC as a result of the photonic bandgap coupling with the excitation light and/or emission light. Depending on the design of the silk fluorescence collimator, the emission can reach 49.37 times higher than the control. The silk fluorescence collimator can be applied to achieve significant benefits: for instance, as a humidity sensor, it provides good reproducibility and a sensitivity of 28.50 a.u./% relative humidity, which is 80.78 times higher than the sensitivity of the control, and as a novel curtain, it raises the energy conversion efficiency of the semitransparent dye-sensitized solar cells (DSSCs) by 16%.@en