A novel metallosupramolecular polypseudorotaxane constructed by metal coordination and pillar[6]arene-based molecular recognition was built. First, a [2]pseudorotaxane based on a mono(ethylene oxide) substituted pillar[6]arene P6 and a paraquat derivative guest G was prepared. Then Ag⁺ was used to fabricate the metallosupramolecular polypseudorotaxane based on a metal coordination polymer backbone.