In the present study, the processing and the mechanical properties of new t
hermoset nanocomposites prepared from aqueous suspensions of microcrystalli
ne cellulose fillers and epoxy are described. The nature of cellulose fiber
s, which display a large aspect ratio and the ability to associate by means
of H-bonds implies that the processing method chosen in this study avoids
the problem of a high level of viscosity of the epoxy reactive system-whisk
ers mixture. The reinforcing effect of this type of natural fiber in an epo
xy matrix is mainly shown from the dynamic mechanical properties in the rub
bery state. This unusual reinforcement is due to (i) the strong interaction
s existing between the cellulose whiskers and the epoxy network and, (ii) t
he creation of a percolating network linked by H-bonds between cellulose fi
bers. The existence of such a percolation effect is evidenced from the anal
ysis of the rubbery shear modulus of nanocomposites based on various volume
fractions of whiskers with mechanical modeling such as Halpin-Kardos and p
ercolation approaches.