The spatial variations of the gas-to-dust ratio (GDR) provide constraints on the chemical evolution and lifecycle of dust in galaxies. We examine the relation between dust and gas at 10-50 pc resolution in the Large and Small Magellanic Clouds (LMC and SMC) based on Herschel far-infrared (FIR), H I 21 cm, CO, and Halpha observations. In the diffuse atomic ISM, we derive the gas-to-dust ratio as the slope of the dust-gas relation and find gas-to-dust ratios of 380+250-130 in the LMC, and 1200+1600-420 in the SMC, not including helium. The atomic-to-molecular transition is located at dust surface densities of 0.05 Mo pc-2 in the LMC and 0.03 Mo pc-2 in the SMC, corresponding to AV ~ 0.4 and 0.2, respectively. We investigate the range of CO-to-H2 conversion factor to best account for all the molecular gas in the beam of the observations, and find upper limits on XCO to be 6x1020 cm-2 K-1 km-1 s in the LMC (Z=0.5Zo) at 15 pc resolution, and 4x 1021 cm-2 K-1 km-1 s in the SMC (Z=0.2Zo) at 45 pc resolution. In the LMC, the slope of the dust-gas relation in the dense ISM is lower than in the diffuse ISM by a factor ~2, even after accounting for the effects of CO-dark H2 in the translucent envelopes of molecular clouds. Coagulation of dust grains and the subsequent dust emissivity increase in molecular clouds, and/or accretion of gas-phase metals onto dust grains, and the subsequent dust abundance (dust-to-gas ratio) increase in molecular clouds could explain the observations. In the SMC, variations in the dust-gas slope caused by coagulation or accretion are degenerate with the effects of CO-dark H2. Within the expected 5--20 times Galactic XCO range, the dust-gas slope can be either constant or decrease by a factor of several across ISM phases. Further modeling and observations are required to break the degeneracy between dust grain coagulation, accretion, and CO-dark H2.
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