Pre-harvest sprouting (PHS) severely reduces rice grain yield, significantly affects grain quality, and leads to substantial economic loss. In this study, we aimed to characterize the physicochemical properties and processing quality of the Garumi 2 flour rice variety under PHS conditions and compare them with those of the Seolgaeng, Hangaru, Shingil, and Ilpum rice varieties and the Keumkang wheat variety. Analysis of the molecular structure of starch revealed uniform starch granules, increased proportions of short-chain amylopectin in DP 6–12 (51.0–55.3%), and enhanced crystallinity (30.7–35.7%) in rice varieties for flour compared with the Ilpum cooking rice variety. PHS significantly altered the starch structure and gelatinization properties of Garumi 2. It also caused surface pitting and roughness in Garumi 2 starch granules and decreased their crystallinity. Collectively, the findings of this study provide important novel insights into the effects of PHS on the physicochemical properties of Garumi 2 floury rice for flour.