This study investigates the influence of polyol compounds (sorbitol and erythritol) on the osmotic dehydration process of pomegranate seeds. The efficacy of the osmotic dehydration process was estimated based on the determination of water loss, weight reduction, solid gain, and effective diffusivity and also through a comparison of the results obtained between sucrose and polyol osmotic solutions. Response surface methodology was used to optimize the osmotic process. Quality attributes of pomegranate seeds were determined through the assessment of physical (texture and color) characteristics. This innovative research applies alternative solutions in the osmotic process, which until now, have not been commonly used in the osmotic dehydration of pomegranate seeds processing by researchers worldwide. Results revealed the excellent correlation of experimental values with the model. Erythritol and sorbitol exhibit stronger efficiency than sucrose. However, erythritol was not satisfactory due to the high solid gain. Therefore, the sorbitol osmotic agent seems to be the most suitable for the osmotic dehydration of pomegranate seeds. The optimal condition for maximum water loss (38.61%), weight reduction (37.77%), and effective diffusivity (4.01 × 10−8 m2/s) and minimum solid gain (−0.37%) were 13.03 min, 27.77 °Brix, and 37.7 °C, using a sorbitol solution. Results of texture and color revealed the major impact of erythritol and sorbitol osmotic agents on seed characteristics during the osmotic dehydration process.