We report the detailed experimental study on the production of electron-spin-polarized Sr+ ions through one-photon resonant two-photon ionization via laser-excited 5s5p P-3(1) (M-J=+1) of Sr atoms produced by laser-ablation. We have experimentally confirmed that the use of laser-ablation for the production of Sr atoms prior to photoionization does not affect the electron-spin polarization. We have found that the degree of electron-spin polarization is 64+/-9%, which is in good agreement with our recent theoretical prediction. As we discuss in detail, we infer, from a simple analysis, that photoelectrons, being the counterpart of electron-spin-polarized Sr+ ions, have approximately the same degree of electron-spin polarization. Our experimental results demonstrate that the combined use of laser-ablation technique and pulsed lasers for photoionization would be a compact and effective way to realize a pulsed source for spin-polarized ions and electrons for the studies of various spin-dependent dynamics in chemical physics. (C) 2004 American Institute of Physics.