The unique biosignature of life on Earth is the homochirality of organic compounds, such as amino acids, proteins, and sugars. High-energy spin-polarized (spinup or spindown) electrons (SPEs) from the β decay of radioactive nuclei have been proposed as a source of symmetry breaking, leading to homochirality; however, their exact role is much debated. Here, we propose magnetically aligned dust grains as a new source of SPEs, due to the photoemission of electrons having aligned spins by the Barnett effect. For the interstellar UV radiation field of strength G
UV, we find that the SPE emission rate is
Γ
pe
SPE
∼
10
−
14
G
UV
electrons per second per H, the fraction of spin-polarized to total photoelectrons is ∼10%, and the SPE yield (photoelectron number per UV photon) can reach ∼1%, using the modern theory of grain alignment. SPEs emitted from aligned grains could play an important role in chiral-induced spin-selectivity-driven reduction chemistry in the icy grain mantles, producing an enantiomer excess of chiral molecules formed on the grain mantle. Finally, we suggest magnetically aligned grains could directly impact the enantio-selectivity through the chiral-induced spin-selective adsorption effect and exchange interaction. We estimate the disalignment of electron spins and depolarization by elastic scattering using the Mott theory and find that these effects are negligible for low-energy SPEs, so that the spins of SPEs remain well aligned during their journey through dust grains and the gas. Our proposed mechanism might explain the chiral asymmetry of prebiotic molecules detected in numerous comets, asteroids, and meteorites.