A novel layered calcosilicate ( CAS-1) was employed to immobilize an iron-based diimine catalyst 2,6-bis[1-(2,6-diisopropylphenylimino)ethyl]pyridine iron chloride ( I) onto it to form a supported catalyst ( CC) for the first time. The crystal structure of CAS-1 was determined by X-ray crystallographic analysis in addition to SEM characterization. The CC-catalyzed ethylene polymerization exhibited good catalytic activities with either co-catalyst methylaluminoxane (MAO) or triethylaluminum (TEA). The resulting polyethylenes possessed not only higher molecular weight, melting temperature ( T m), and decomposition onset temperature ( T onset) than those obtained with its homogeneous counterpart, but also a unique morphology.