This investigation reports on the thermomechanical properties of Poly-tripropyleneglycoldiacrylate (Poly-TPGDA)/liquid crystal (LC) blends, developed via free radical polymerization processes, which are induced by Electron Beam (EB) and Ultraviolet (UV) radiation. The EB-cured Poly-TPGDA network exhibits a higher glass transition temperature (Tg), a higher tensile storage, and Young moduli than the corresponding UV-cured sample, indicating a lower elasticity and a shorter distance between the two adjacent crosslinking points. Above Tg of Poly-TPGDA/LC blends, the LC behaves as a plasticizing agent, whereas, for EB-cured networks, at temperatures below Tg, the LC shows a strong temperature dependence on the storage tensile modulus: the LC reinforces the polymer due to the presence of nano-sized phase separated glassy LC domains, confirmed by electron microscopy observations. In the case of the UV-cured TPGDA/LC system, the plasticizing effect of the LC remains dominant in both the whole composition and the temperature ranges explored. The rubber elasticity and Tg of Poly-TPGDA/LC films were investigated using mechanical measurements.