Natural nacre with superior mechanical property is generally attributed to the layered “brick-and-mortar” nanostructure. However, the role of nanograins on the hard aragonite platelets, which is so-called nanoasperity, is rarely addressed. Herein, we prepared silica platelets with aragonite-like nanoasperities via biomineralization strategy and investigated the effects of nanoasperity on the mechanical properties of resulting layered nanocomposites composed of roughened silica platelets and poly(vinyl alcohol). The tensile deformation behavior of the nanocomposites demonstrates that nanograins on silica platelets are responsive for strain hardening, improved strength, and toughness. The structure origin is attributed to the nanoasperity-controlled platelet sliding.