We have determined column densities of H I and/or H 2 for sight lines in the Magellanic Clouds from archival HST and FUSE spectra of H I Lyman-α and H 2 Lymanband absorption. Together with some similar data from the literature, we now have absorption-based N (H I) and/or N (H 2 ) for 285 LMC and SMC sight lines (114 with a detection or limit for both species) -enabling more extensive, direct, and accurate determinations of molecular fractions, gas-to-dust ratios, and elemental depletions in these two nearby, low-metallicity galaxies. For sight lines where the N (H I) estimated from 21 cm emission is significantly higher than the value derived from Lyman-α absorption (presumably due to emission from gas beyond the target stars), integration of the 21 cm profile only over the velocity range seen in Na I or H 2 absorption generally yields much better agreement. Conversely, N (21 cm) can be lower than N (Ly-α) by factors of 2-3 in some LMC sight lines -suggestive of small-scale structure within the 21 cm beam(s) and/or some saturation in the emission. The mean gas-to-dust ratios obtained from N (H tot )/E(B − V ) are larger than in our Galaxy, by factors of 2.8-2.9 in the LMC and 4.1-5.2 in the SMC -i.e., factors similar to the differences in metallicity. The N (H 2 )/E(B − V ) ratios are more similar in the three galaxies, but with considerable scatter within each galaxy. These data may be used to test models of the atomic-to-molecular transition at low metallicities and predictions of N (H 2 ) based on comparisons of 21 cm emission and the IR emission from dust. a Entries marked with an asterisk include contributions from another weak, isolated component. b Column density integrated over full extent of 21 cm profile. c Column density integrated over limited range in velocities seen in Na I absorption (extended by 5 km s −1 at both ends).