File Name : figure s1a.tif

Caption : figure s1a.  atomic structures of the ti₃c₂tₓ mxene models used in this work, including ti₃c₂, ti₃c₂o₂, and ti₃c₂(oh)₂.

File Name : figure s1b.tif

Caption : figure s1b. three-dimensional representations of the silk fibroin (sf) molecular structure from different viewing orientations.

File Name : figure s2a.tif

Caption : figure s2a. layered architecture of mxene (ti3c2)/sf composites with varied chain orientations. the illustrations depict the mxene nanosheets interleaved with sf chains oriented at a) 0° (parallel), b) 45° (diagonal), c) 90° (perpendicular), relative to the mxene surface.

File Name : figure s2b.tif

Caption : figure s2b. layered architecture of mxene (ti3c2o2)/sf composites with varied chain orientations. the illustrations depict the mxene nanosheets interleaved with sf chains oriented at a) 0°, b) 45°, c) 90° relative to the mxene surface.

File Name : figure s2c.tif

Caption : figure s2c. layered architecture of mxene (ti3c2(oh)2)/sf composites with varied chain orientations. the illustrations depict the mxene nanosheets interleaved with sf chains oriented at a) 0°, b) 45°, c) 90° relative to the mxene surface. 

File Name : figure s3.tif

Caption : figure s3. structural integrity of silk fibroin (sf) during shear deformation. dssp analysis of the secondary structure composition for sf layers in different mxene/sf composites across 0°, 45° and 90° orientations.

File Name : figure s4.tif

Caption : figure s4. synergistic effects of mxene surface functionalization and silk fibroin alignment angle on the mechanical performance and its interfacial failure modes.

File Name : table s1.tif

Caption : table s1. the water molecular number in different systems.