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Polarized electron-deuteron deep-inelastic scattering (DIS) with detection of the spectator proton (“tagged DIS”) enables measurements of neutron spin structure with maximal control of nuclear effects. We calculate the longitudinal spin asymmetries in polarized tagged DIS using methods of light-front nuclear structure and study their dependence on the measured proton momentum. Asymmetries can be formed with all three deuteron spin states (±1,0) or the two maximum-spin states only (±1, involving tensor polarization). The proton momentum dependence can be used to select pure S-wave configurations in the deuteron and eliminate D-wave depolarization (transverse momenta ppT≲ 100 MeV). Free neutron spin structure can be extracted model-independently through pole extrapolation of the tagged asymmetries. Such measurements could be performed at a future electron-ion collider (EIC) with polarized deuteron beams and forward proton detectors. Keywords: Polarized deep-inelastic scattering, Neutron, Nuclear fragmentation, Electron-ion collider, Light-front quantization