SnS is an environmentally friendly, cost-effective, and earth-abundant narrow-bandgap semiconductor with substantial potential for medium-temperature thermoelectric applications. However, the thermoelectric performance of its bulk counterpart is inherently constrained by intrinsic point defects (e.g., vacancies) and the material’s specific band structure. Low-dimensional engineering has emerged as a pivotal strategy for overcoming these limitations and enhancing thermoelectric performance. In this work, we systematically investigate the thermoelectric properties of SnS nanofilms with distinct thicknesses (82 nm, 199 nm, 616 nm, and 813 nm) across a temperature range of 300–600 K. Measurements were conducted using time-domain thermoreflectance (TDTR) and a dedicated thin-film thermoelectric parameter test system (ZEM-3). Our results confirm that low-dimensionalization effectively boosts the thermoelectric performance of SnS, with the thermoelectric figure of merit (ZT) displaying a pronounced dependence on both film thickness and temperature. All four SnS thin films exhibit thermoelectric performance that is markedly superior to that of bulk SnS. This enhancement is primarily attributed to the quantum confinement effect, energy filtering effect, and intensified phonon scattering, all of which are induced by the low-dimensional structural characteristics. This work provides not only experimental evidence and theoretical insights for the performance optimization of SnS nanofilms but also establishes a foundational framework for the development of high-efficiency, eco-friendly medium-temperature thermoelectric materials, thereby holding significant scientific value and practical implications.