Biodegradable nanocomposites of Nanocrystalline Cellulose (NCC) and electrospun poly-(lactic acid) were prepared via a new mixing technique. Dispersion of hydrophilic NCC in hydrophobic PLA was improved through aqueous mixing and freeze drying of perfectly suspended NCC with PLA nanofibers. Freeze drying produced aerogels with good mechanical integrity. The aerogels were further processed via hot pressing. Resulting composites displayed an improvement in mechanical properties, which was greatest at temperatures below the glass transition temperature of PLA. The optimum compositions were found to be in the 0.5-3% NCC (by weight) range. Experiments performed also showed that due to electrospinning, the crystallinity of the PLA slightly increased and this is accompanied by a decrease in its glass transition temperature. Furthermore, adding NCC to the electrospun PLA matrix did not alter the crystallinity of the final composite. The composites investigated proved their potential to be used in packaging and tissue engineering applications. (c) 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 3345-3354, 2013