We describe the fabrication of physical chitosan hydrogels exhibiting a layered structure. This
bilayered structure, as shown by SEM and confocal microscopy, is composed of a thin dense
superficial zone (SZ), covering a deeper zone (DZ) containing microchannels orientated
perpendicularly to the SZ. We show that such structure favors diffusion of macromolecules
within the hydrogel matrix up to a critical pressure, σc, above which channels were
constricted. Moreover, we found that the SZ provided a higher wear resistance than the DZ
which was severely damaged at a pressure equal to the elastic modulus of the gel. The
coefficient of friction (CoF) of the SZ remained independent of the applied load with μSZ =
0.38 ± 0.02, while CoF measured at DZ exhibited two regimes: an initial CoF close to the
value found on the SZ, and a CoF that decreased to μDZ = 0.18 ± 0.01 at pressures higher than
the critical pressure σc. Overall, our results show that internal structuring is a promising
avenue in controlling and improving the wear resistance of soft materials such as hydrogels