In an attempt to prepare smooth nanostructured thin films of silk fibroin (SF) by near-infrared (NIR) pulsed laser deposition, an opaque target was prepared from an emulsified aqueous solution of SF. Upon irradiation of 1064-nm pulsed laser beam at its fluence 5 J/cm(2), a thin film of SF was deposited on the Si(100) substrate with its root-mean-square surface roughness, 037 nm, smoother than those obtained from a compressed target of SF powders by approximately an order of magnitude. The attainment of an extra-smooth film from the opaque target was discussed in terms of multiple Mie scattering of the incident NIR beam, leading to an increase in the plasma density, intensified optical breakdown, ablation of better dispersed SF molecular units, and a film with more intensive intermolecular cross-linking. (C) 2013 Elsevier B.V. All rights reserved.