In this study, we explored a wide range of green solvents to process the semiconductor layer TIPS-PEN (6,13-bis(triisopropylsilylethynyl)pentacene), as well as to demonstrate potential generality, using several p- and n-type organic semiconductors, for the fabrication of organic thin-film transistors (OTFTs). Our data demonstrate that several different solvents enable good semiconductor film-forming morphologies and optimized TIPS-PEN TFT mobilities of ∼0.5–2 cm² V⁻¹ s⁻¹, thus surpassing those of toxic chlorinated options. Furthermore, we utilized a green cellulose cinnamate-gate dielectric to fabricate TIPS-PEN OTFTs, where both the semiconductor and the dielectric were processed using green solvents demonstrating the feasibility of a more sustainable OTFT technology.