Understanding the origin of chirality in nature has been an active area of research since the time of Pasteur. In this chapter we examine one possible route by which this asymmetry could have arisen, namely chiral-specific chemistry induced by spin-polarized electrons. The various sources of spin-polarized electrons (parity violation, photoemission, and secondary processes) are discussed. Experiments aimed at exploring these interactions are reviewed starting with those based on the Vester–Ulbricht hypothesis through recent studies of spin polarized secondary electrons from a magnetic substrate. We will conclude with a discussion of possible new avenues of research that could impact this area.