A　facile,　environmentally　benign　approach　has　been　developed　for　the　preparation　of　dynamic,　multiresponsive,　and　self-healing　hydrogels　from　inexpensive　bamboo　pulp,　poly(vinyl　alcohol)　(PVA),　and　borax.　The　microfibrillated　cellulose　(MFC)　reinforced　PVA-borax　hydrogels　were　produced　through　a　one-pot　route　in　conjunction　with　ball　milling　and　physical　blending　in　tandem　in　aqueous　medium.　In　this　way,　MFC　particles　could　be　efficiently　generated　and　well-dispersed　in　a　polymer　matrix,　and　they　have　been　verified　by　scanning　electron　microscopy.　The　rheology　analysis　indicated　a　close　relationship　between　the　mechanical　strength　and　the　MFC　loading　and　ball　milling　time.　Due　to　the　dynamic　equilibrium　of　the　didiol-borax　linkages　and　the　reinforcement　of　MFC　fibers,　the　hydrogels　showed　enhanced　self-healing　behavior　and　mechanical　stiffness,　which　was　also　supported　by　rheology　analyses.　In　addition,　the　hydrogels　were　found　to　be　sensitive　to　the　pH　value.　The　hydrogels　present　a　solvent　or　gel　state　with　the　change　of　pH　value,　and　this　sol-gel　transfer　can　be　repeated　while　maintaining　the　shape,　further　demonstrating　the　dynamic　reversible　behavior　of　the　hydrogels.　©　2016　American　Chemical　Society.