The present monograph summarizes, in a comprehensive way, several years of joint experimental and theoretical frontier research on ultrafast laser-induced molecular dynamics and its control. Emphasis is set on the characterization of the nuclear dynamics within molecular systems in various environments (gas phase, surfaces, solids, solution, strong fields) triggered by optical excitations spanning from the infrared to the ultraviolet. Building on the converged analysis between experiment and theory, control of chemical reactions is established by means of optimally shaped laser pulses. This paves the road toward new applications and future challenges in this rapidly developing research field.