Debranching modifications of waxy corn starch with pullulanase can generate short-chain amylose or debranched starch (DBS), which is easy to recrystallize. Herein, we firstly investigated the regulation of recrystallization behaviors of DBS by studying the interactions between DBS and emulsifiers, polyphenols, and fatty acids. Sodium dodecyl sulfate at the 3.0% level had strong interactions with DBS. When the concentration of epigallocatechin gallate was 15%, the enthalpy change (ΔH) of DBS was close to 0 J/g and the relative crystallinity of DBS was 0, clearly indicating the strong interactions between epigallocatechin gallate and DBS. When the concentration of caproic acid, caprylic acid, and capric acid increased from 0 to 20.0%, the ΔH of DBS decreased from 11.38 ± 0.01 to 3.90 ± 0.63, 1.39 ± 0.21, and 3.98 ± 0.83 J/g, respectively. The interactions between emulsifiers, polyphenols, and fatty acids and DBS could affect physiochemical properties of DBS in varying degrees.