Heterogeneous catalysts, as an emerging research hotspot, have showed excellent advantages on stability, reryclability, and separation from reactant compared with homogeneous catalysts in recent years. Herein, pillar[5]-arene-based organometallic cross-linked polymer (P[5]-OCP) was constructed via the complexation between imidazolium-derivatived pillarNarene (P[5]) and Pd(OAc)(2). The chemical compositions and structure of the P[5]-OCP were confirmed by means of multiple characterization methods. The catalytic activity and process of P[5]-OCP were emphatically investigated in the Suzuki-Miyaura coupling reaction. The P[5]-OCP showed outstanding catalytic activity in mild reaction conditions. Meanwhile, the catalyst P[5]-OCP possessed excellent stability and recyclability, which could be reused at least five times without significant loss of activity. Furthermore, the P[5]-OCP is easily synthesized and cost-effective, which make it a candidate for applications in fine chemical engineering.