Functional segmented polymer networks (FSPNs) were synthesised via free radical initiated copolymerisation of polytetrahydrofuran (PTHF) bis-macromonomers with vinylbenzyl chloride (VBCl). The purpose of this work was to create FSPNs, providing supports with a functional group that can be substituted and may serve to immobilise other reagents such as catalysts. After the preparation and detailed characterisation of several PTHF bis-macromonomers, FSPNs were prepared with varying molecular weight of the PTHF chain and varying PTHF/ PVBCl ratio. Measurements of the soluble fraction and elemental analyses demonstrated that FSPNs with a wide composition range could be prepared. From dynamic-mechanical and thermal analyses, it could be concluded that most FSPNs showed some degree of compatibility and complete absence of crystallinity. The mechanical properties of the FSPNs are directly related to their composition. The degree of substitution of all networks is close to quantitative.