Natural products have long served as inspirations and testing grounds for new synthetic methodologies and strategies. They are also valuable sources for lifesaving drug molecules. This talk will highlight elements of our recent efforts in developing novel strategies and methodologies for divergent and efficient synthesis of medicinally important natural products. Particular emphasis will be placed on two research projects. One will focus on our discoveries of tandem catalytic carbonylation reactions for the total syntheses of macrolides and spirocyclic natural products.