Currently, high strength nacre-inspired PVA/MMT (polyvinyl alcohol/montmorillonite) nanocomposites with high MMT nanofiller content (50-70 wt%) have been constructed successfully. However, this seriously sacrifices the elongation and reduces the corresponding transparency. In this paper, high elongation and transparent PVA/MMT nanocomposites with high MMT content are prepared by the evaporation-induced assembly with the introduction of the micro-crosslinking. Results demonstrate that the micro-crosslinking can inhibit the formation of rod-shaped arrays, and contribute to a more ordered layered microstructure, where an elongation of 76.2% in 47.8 wt% MMT content nanocomposites is gained, nearly 19 times of that of non-crosslinked nanocomposites (ultimate strain is 4.1%). This provides a potential approach for compromise between high strength and excellent elongation at the same MMT content. Moreover, disappearance of rod-shaped arrays and resultant ordered layered microstructure make eventual films more transparent.