Polypseudorotaxane-based 3D-printing hydrogels consisting of dimethacrylamide-poly(ethylene-glycol) and α-CD have been developed. After post-printing crosslinking, the 3D-printed polyrotaxane monolith exhibits rapid and reversible shape morphing upon pH variation. Copolymerization of the polypseudorotaxane with acrylates affords hybrid 4D printing materials that are responsive to pH and ionic strength.