Owing to their apparent lack of health significance, higher straight-chain aliphatic aldehydes, i.e., those having alkyl chains with more than six carbon atoms, have been largely neglected in food and nutraceutical research. However, they are an important class of odor-active volatiles in human foods. Indeed, certain aldehydes, such as hexanal, E-2-nonenal, and E,E-2,4decadienal, serve as key odorants in a range of our foods and drinks. This perspective describes the significance of higher straight-chain aliphatic aldehydes as food odorants, focusing on several representative ones, and raises the issues regarding these aldehydes to be addressed in the future.