The preparation of a printable silicon ink using semiconductor grade and commercially available trisilane (Si3H8) is reported. The synthesis is carried out in solution at room temperature or below in N2 atmosphere at ambient pressure and involves an initial sonication step, followed by irradiation with ultraviolet light. The production of higher order silanes via ultrasound is demonstrated using gas chromatography and nuclear magnetic resonance measurements are used to show that a combined sonophotolytic treatment yields a highly branched silicon hydride polymer. In addition, scanning electron microscopy (SEM) images are used to ascertain the sonocatalytic production of silicon nanoparticles. Furthermore, it is argued that these particles are partially responsible for enabling dramatically accelerated polymer growth, not otherwise observed in the same amount of time using ultraviolet light alone. Finally, the utility of the ink used in this study is demonstrated for the field of printable electronics by fabricating amorphous silicon thin films by spin‐coating and atmospheric pressure chemical vapor deposition with optoelectronic properties approaching those of state‐of‐the‐art plasma enhanced chemical vapor deposition (PECVD) material.