Triboelectricity and triboluminescence of materials are utilized in the development of structural health monitoring systems. The triboelectric phenomenon was first reported in 2012 with the invention of triboelectric nanogenerators (TENGs). The working principle of TENGs is based on the contact electrification and electrostatic induction. As a result of the periodic contact and separation of these two materials, TENGs convert the mechanical energy, such as vibration, acceleration, and wind etc., into electricity. Triboluminescent (TL) crystals emit light under mechanical force and they are generally used in mechanosensor applications. In this study, polymer composite material composed of Poly(vinylidene fluoride) (PVDF) thin film and organometallic crystal, europeum tetrakis triethyl ammonium chloride (EuD4TEA) were prepared. The electrical and optical performance of the resulting composite system was measured simultaneously with a homemade device.