Self-oscillating synthetic vocal fold (VF) models are often used to study human voice production. In this thesis, a method for fabricating multi-layer self-oscillating synthetic VF models using silicone 3D printing is presented. Multi-material 3D printing enables faster fabrication times with more complex geometries than traditional casting methods and builds a foundation for producing VF models with potentially more life-like geometries, materials, and vibratory characteristics. The printing method in this study used a custom dual extruder and slicing software to print UV-curable liquid silicone into a gel-like support matrix. The extruder was fabricated using high-torque stepper motors with high resolution leadscrews for precise extrusion and retraction. The custom slicing software accounted for challenges with printing a low-viscosity uncured silicone and was capable of allowing the user to visually observe the effects of print settings on print paths before finalizing the g-code. Three validation tests were conducted to demonstrate the 3D printer’s ability to print ultra-soft silicone with the desired range of stiffness, change between materials quickly, and print a material stiffness gradient. Two types of VF models were printed in this study, a previously-designed model with multiple distinct layers (“EPI” model), and the same model but with a vertical stiffness gradient (VSG) in the superficial lamina propria layer. The EPI model was chosen to demonstrate the ability to 3D print a multi-layer model, and the VSG model was chosen to demonstrate the ability to print multi-material VFs with geometric and material properties that are difficult to fabricate using traditional casting methods. Sixteen VFs (i.e., eight pairs) of each model type were printed, and their vibratory responses were recorded, including onset pressure, frequency, and glottal width. A micro-CT scanner was used to evaluate the external geometric accuracy of the models. One-centimeter cubes were 3D printed and tensile tested to characterize the material properties of each set of VF models. The material and phonatory properties of both the EPI and VSG VF models were found to be comparable to human data and to previous data acquired using synthetic VF models fabricated via other methods. In this thesis, the 3D printing methodology is summarized, the setup and results of the validation and VF model tests are reported and discussed, and recommendations for future work are provided.