Silicon nanoparticles (SiNPs) can be challenging to prepare with defined size, crystallinity, composition, and surface chemistry. As is the case for any nanomaterial, controlling these parameters is essential if SiNPs are to realize their full potential in areas such as alternative energy generation and storage, sensors, and medical imaging. Numerous teams have explored and established innovative synthesis methods, as well as surface functionalization protocols to control these factors. Furthermore, substantial effort has been expended to understand how the abovementioned parameters influence material properties. In the present review we provide a commentary highlighting the benefits and limitations of available methods for preparing silicon nanoparticles as well as demonstrations of tailoring optical and electronic properties through definition of structure (i.e., crystalline vs. amorphous), composition and surface chemistry. Finally, we highlight potential opportunities for future SiNP studies.