During the process of direct-ink-write (DIW) 3D printing, the extrusion shear force can be leveraged to fabricate structures with filaments featuring a bioinspired concentric lamellar microstructure. Based on this novel approach, this poster showcases the design and fabrication of bioinspired inorganic-organic composite materials with synergistic mechanical and functional enhancement. In one study, ceramic nanocomposites with a high inorganic content (95 wt.%) and a minimal organic phase are prepared, which reveal excellent flexibility for shape morphing owing to their concentric lamellar microstructure. These flexible ceramic nanocomposites can be used in 4D printing through a programmable prestrain approach to deform into complex structures hardly achievable with conventional 3D printing. In another study, a novel bioceramic nanosheet material called "BCene" is developed via selective demetallization of Akermanite bioceramics. Through DIW 3D printing, flexible and robust bioceramic nanosheet composite scaffolds are developed with both enhanced mechanical and biological performance. In summary, this poster presents the shear-induced alignment technique via DIW 3D printing and investigates the mechanical and functional properties of the 3D printed bioinspired composite materials. The findings shall contribute to the research of bioinspired materials fabrication from material synthesis to structural technologies like 3D printing.