We have determined column densities of H I and/or H_2_ for sight lines in the Magellanic Clouds from archival Hubble Space Telescope and Far-Ultraviolet Spectroscopic Explorer spectra of H I Ly{alpha} and H_2_Lyman-band absorption. Together with some similar data from the literature, we now have absorption-based N(H I) and/or N(H_2_) for 285 Large Magellanic Cloud (LMC) and Small Magellanic Cloud (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 Ly{alpha} 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{alpha}) 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.