Marine mussels use their threads for attachment to any substratum and these biopolymer gradient fibers show an excellent combination of stiff and soft mechanical properties. A straightforward approach for the preparation of macroscopic longitudinal polymer gradient materials on the centimeter scale based on a poly(dimethyl siloxane) system is presented. Compositional gradients are realized by using three syringe pumps feeding different prepolymers capable to undergo thermal cross-linking. Within the gradient samples, the stiffness between the hard and soft part can be varied up to a factor of four. The gradients are analyzed by UVVis spectroscopy as well as compressive and tensile modulus testing.