© 2021 American Chemical Society.Rare sugars are monosaccharides and their derivatives that are not commonly found in nature. d-Allulose is a rare sugar that is C-3 epimer of fructose and presents an alternative to sucrose with potential health benefits. In this study, different amounts of sucrose, d-allulose, and soy protein isolate (SPI) were used to prepare a set of pectin gels. The effect of these ingredients on the gels was studied at both a molecular level, by 1H nuclear magnetic resonance (NMR) relaxometry, and a macroscopic level, through the assessment of viscoelastic properties as well as hardness and moisture content measurements. The NMR dispersion profiles were analyzed considering relaxation mechanisms associated with rotational and translational diffusion motions of mono- and disaccharides as well as bound water molecules. Significant variations of the local diffusion coefficient for the studied formulations were evidenced by the model fitting analysis. The viscosity trends observed within each group of samples having the same amount of SPI were mostly in agreement with the diffusion coefficients obtained from the NMR relaxometry. The observed discrepancies could be explained considering hardness and moisture content results, which put into evidence the fact that decreasing the moisture (mainly free water) affects the macroscopic properties of the systems, such as hardness and viscosity, but not the local diffusion processes probed by NMR relaxometry. These findings show the importance of combining both micro- and macroscopic information to analyze the different properties of food products.