Sulfur-bearing Fe-rich nanoparticles (SINPs) have been subject to increased levels of interest because of their catalytic properties and other features. However, with increasing interest in greener and sustainable practice, traditional engineered routes to SINP synthesis have become a concern owing to their high energy and resource demand as well as the use of potentially hazardous or environmentally harmful reagents. Here, we aim to bring attention to emerging and burgeoning research across a wide range of disciplines on the formation of both naturally occurring and synthetic SINPs. First, various SINP types are described, and their most important characteristics are outlined. Second, the natural mechanisms of SINP formation are evaluated and their environmental significance explained, predominantly in hydrothermal vents and lithogenic environments, in order to help inspire new approaches to engineered synthesis. Third, an appraisal of various synthetic approaches for SINP assembly is presented, with a focus on green synthesis methods. One exemplar is the use of nature inspired biosynthesis, which has been increasingly explored for the fabrication of cost-effective and environmentally friendlier SINPs. Finally, potential future research directions leading to more sustainable SINP synthesis are put forward.