Recent advances in digital workflow have transformed clinician's ability to offer patient-specific devices for medical and dental applications. However, the digital workflow of patient-specific maxillofacial prostheses (MFP) remains incomplete, and several steps in the manufacturing process are still labor-intensive and are costly in both time and resources. Despite the high demand for direct digital MFP manufacturing, three-dimensional (3D) printing of colored silicone MFP is limited by the processing routes of medical-grade silicones and biocompatible elastomers. In this study, a binder jetting 3D printing process with polyvinyl butyral (PVB)-coated silicone powder was developed for direct 3D printing of MFP. Nanosilica-treated silicone powder was spray dried with PVB by controlling the Ohnesorge number and processing parameters. After printing, the interconnected pores were infused with silicone and hexamethyldisiloxane (HMDS) by pressure-vacuum sequential infiltration to produce the final parts. Particle size, coating composition, surface treatment, and infusion conditions influenced the mechanical properties of the 3D-printed preform, and of the final infiltrated structure. In addition to demonstrating the feasibility of using silicone powder-based 3D printing for MFP, these results can be used to inform the modifications required to accommodate the manufacturing of other biocompatible elastomeric materials.