The applications of sugars as inexpensive, renewable, and nontoxic sources of hydrogen gas are systematically demonstrated by means of dehydrogenation and catalytic transfer hydrogenation reactions. The chiral bifunctional Noyori‐type catalyst, Cp*Ir(TsDPEN), is found to effectively, regioselectively, and stereoselectively dehydrogenate various sugars possessing different steric hindrance and stereochemistry. Furthermore, kinetics experiments for these dehydrogenation reactions reveal that many sugars are superior sources of hydrogen gas when compared with a traditional hydrogen donor, isopropanol. Applications of sugars in transfer hydrogenation with various hydrogen acceptors are also investigated.