A novel picosecond-laser pulsed laser deposition method has been developed for fabricating functionally graded films with pre-designed gradient profiles. Theoretically, the developed method is capable of precisely fabricating films with any thicknesses and any gradient profiles by controlling the laser beam powers for the two different targets based on the film composition profiles. As an implementation example, we have successfully constructed functionally graded diamond-like carbon films with six different gradient profiles: linear, quadratic, cubic, square root, cubic root, and sinusoidal. Energy dispersive X-ray spectroscopy is employed for investigating the chemical composition along the thickness of the film, and the deposition profile and thickness errors are found to be less than 3% and 1.04%, respectively. To the best of the authors' knowledge, this is the first method for fabricating films with designed gradient profiles and has huge potential in many areas of coatings and films, including multifunctional optical films. We believe that this method is not only limited to the example considered in this study, but also can be applied to all material combinations as long as they can be deposited using the pulsed laser deposition technique.