Herein, we fabricated a hybrid PDVB-Ln4L4 metallopolymer using a vinyl functionalized lanthanide-organic tetrahedral cage as the cross-linking agent. Such a covalent embedding strategy not only tunes the morphology and porosity of the metallopolymer, but also improves the luminescence property of the lanthanide organic polyhedron. Potential application in lanthanide separation has also been demonstrated. This study provides a potential strategy for the immobilization of multinuclear lanthanide-organic edifices toward heterogeneous application.