This work reports on the combination of polyhydroxyalkanoate (PHA)-based materials and nanokeratin extracted from poultry feathers (a food by-product) using different approaches. In the first approach, high-barrier nanobiocomposites based on the combination of PHAs with a nanokeratin additive were successfully developed via both (i) direct melt compounding and (ii) prein-corporated into an electrospun masterbatch of PHA which was subsequently melt compounded with PHA pellets. Enhanced barrier properties for the nanobiocomposites were obtained which were seen to depend on the PHA grade used. In the second approach, nanokeratin films were obtained via solution casting which were successfully hydrophobized by coating them with electrospun PHA fibers. The multilayered approach showed good adhesion and also lead to enhanced barrier performance. (C) 2015 Wiley Periodicals, Inc.