This work investigated the potential of improving flexural properties of natural fiber (jute) reinforced biocomposites by atmospheric pressure helium plasma treatment. Composites were made by the use of combined hand lay-up and vacuum bagging technique followed by newly developed Australia patented QuickstepTM curing. The physical properties of helium plasma modified fibers were investigated by means of wettability time, coefficient of friction (COF), atomic force microscopy (AFM) and chemical nature of the surface with ATR-FTIR and XPS. There was found a logical correlation between physical and chemical characteristics of the surface of fiber with the fracture mechanical behavior of their resulting biocomposites. In addition, the use of helium atmospheric plasma treatment prior to QuickstepTM process has proved to be a potential way to positively alter the fracture-mechanical behavior of biocomposites. This study will lead to new commercial applications of natural fiber jute for the composite industry that go beyond wrapping and packaging.