Hydrothermal synthesis of surface-modified magnetite nanoparticles (NPs) was performed in a batch reactor at 200 °C for 20 min while using monocarboxylic acid with various alkyl chain lengths (C6 to C18) as surface modifiers. The short-chain cases (C6 to C12) successfully gave the surfacemodified NPs with uniform shape and magnetite structure, while the long-chain cases (C14 to C18) gave the NPs with nonuniform shape and two structures (magnetite and hematite). Additionally, the synthesized NPs were revealed to have single crystallinity, high stability, and ferromagnetic property, which were useful for hyperthermia therapy via various characterization techniques. These investigations would guide the selection guidelines for a surface modifier to control the structure, surface, and magnetic properties of surface-modified magnetite NPs with high crystallinity and stability, particularly for hyperthermia therapy applications.