Polyurethanes (PUs) are one of the most versatile polymers and are widely used in our daily lives for rigid and flexible foams, coatings, films, and other products. PUs are generally synthesized through reactions between isocyanates and polyols. A brief overview of the chemical structures, origin, synthetic methods, and properties of polyols and isocyanates is given in this chapter. Currently, most polyols are petroleum-based, but increasing concerns over the depletion of petroleum resources, environment, and sustainability have led to considerable efforts to develop bio-based polyols and PUs from renewable resources. Bio-based polyols and isocyanates for the production of bio-based PUs are discussed in this chapter.