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We show that significant electronic and nuclear polarizations of 31P donors in highly enriched 28Si can be obtained by dynamic optical pumping. Polarization of the donor spins is observed using photoluminescence excitation spectroscopy and optical pumping of individual hyperfine components of the 31P bound exciton transition. Previous samples of 28Si used for 31P bound exciton spectroscopy were p-type due to excess boron, while more recently, samples of 31P-doped n-type 28Si with 99.99% isotopic purity became available. The selective pumping and ionization of 31P donors in specific electronic and nuclear spin states has applications in quantum computing, where a highly polarized initial state is required. [ABSTRACT FROM AUTHOR]