As a special kind of supramolecular compound with many favorable properties, pillar[n]arene-based supramolecular polymer networks (SPNs) show potential application in many fields. Although we have come a long way using pillar[n]arene to prepare SPNs and construct a series of smart materials, it remains a challenge to enhance the mechanical strength of pillar[n]arene-based SPNs. To address this issue, a new supramolecular regulation strategy was developed, which could precisely control the preparation of pillar[n]arene-based SPN materials with excellent mechanical properties by adjusting the polymer network structures. Specifically, we utilized the host-guest interaction between pillar[5]arene and the alkyl chain of butyl acrylate monomer to form a supramolecular polymer network and achieved the transformation of different states by regulating the cross-linking density of the polymer networks. Additionally, the polymer networks exhibited good stimuli responsiveness as well as excellent dynamic properties and reconfigurable characteristics through a temperature change and the addition of competitive hosts or guests. The research provided new possibilities for the development of polymer materials.