Harnessing cost-efficient printable semiconductor materials as near-infrared (NIR) emitters in light-emitting diodes (LEDs) is extremely attractive for sensing and diagnostics, telecommunications, and biomedical sciences. However, the most efficient NIR LEDs suitable for printable electronics rely on emissive materials containing precious transition metal ions (such as platinum), which have triggered concerns about their poor biocompatibility and sustainability. Here, we review and highlight the latest progress in NIR LEDs based on non-toxic and low-cost functional materials suitable for solution-processing deposition. Different approaches to achieve NIR emission from organic and hybrid materials are discussed, with particular focus on fluorescent and exciplex-forming hostguest systems, thermally activated delayed fluorescent molecules, aggregation-induced emission fluorophores, as well as lead-free perovskites. Alternative strategies leveraging photonic microcavity effects and surface plasmon resonances to enhance the emission of such materials in the NIR are also presented. Finally, an outlook for critical challenges and opportunities of non-toxic NIR LEDs is provided.