Biofabrication is the process of transforming materials into systems that reproduce biological structure and function. Previous attempts to create biomimetic systems have often used single materials shaped into limited configurations that do not mimic the heterogeneous structure and properties of many biological tissues. The identification of new bio-inspired materials alongside the development of appropriate fabrication techniques is the key to overcoming the challenge of replicating the functional gradients of these heterogeneous tissues. This paper presents a new extrusion-based gradient printing system that utilizes custom software to control the rates at which two inks are dispensed through a mixing nozzle. The printer was used to fabricate a range of composite materials containing varying blends of a tough alginate/poly(acrylamide) ionic covalent entanglement hydrogel and an acrylated urethane based UV-curable adhesive material. The hard adhesive material acted as particulate reinforcement within the matrix of composites printed with a large hydrogel volume fraction. The composite materials were characterized mechanically and their performance could be modeled with standard composite theory. The platform of a 3D printer allowed these composite materials to be fabricated directly with a smooth and continuous gradient of modulus between the soft hydrogel and harder acrylated urethane material, which may be useful in the development of bio-inspired structures such as artificial tendons.