Multi-head 3D printers afford the ability to create composite structures with significant differences in properties compared to those created through traditional molding techniques. In addition to the usage of different viscoelastic polymeric materials, the selective spatial placement of the build materials enables the creation of layered and graded geometries to achieve specific mechanical and/or vibrational characteristics. This paper describes how the mechanical properties of the individual materials can be used to predict the damping and natural frequencies of a 3D-printed graded structure. Such structures can find usage in rotating machinery, beams, etc., where vibrational characteristics must be controlled. The simulation and experimental results are presented and two forms of the storage and loss modulus are considered: fixed and variable. For the latter condition, E′ and E″ are established as functions of temperature and frequency. Modal vibration testing of the graded samples shows a good match between the simulation and experimental trials, thereby supporting the proposed model as a useful tool for prescribing the structure of a printed part with tailored dynamic properties.