Carbon nanomaterials is among the most promising technologies for advanced electronic applications, due to their extraordinary chemical and physical properties. Nonetheless, after more than two decades of intensive research, the application of carbon-based nanostructures in real electronic and optoelectronic devices is still a big challenge due to lack of scalable integration in microelectronic manufacturing. Laser processing is an attractive tool for graphene device manufacturing, providing a large variety of processes through direct and indirect interaction of laser beams with graphene lattice: functionalization, oxidation, reduction, etching and ablation, growth, etc. with resolution down to the nanoscale. Focused laser radiation allows freeform processing, enabling fully mask-less fabrication of devices from graphene and carbon nanotube films. This concept is attractive to reduce costs, improve flexibility, and reduce alignment operations, by producing fully functional devices in single direct-write operations. In this paper, a picosecond laser with a wavelength of 515 nm and pulse width of 30 ps is used to pattern carbon nanostructures in two ways: ablation and chemical functionalization. The light absorption leads to thermal ablation of graphene and carbon nanotube film under the fluence 60-90 J/cm2 with scanning speed up to 2 m/s. Just under the ablation energy, the two-photon absorption leads to add functional groups to the carbon lattice which change the optical properties of graphene. This paper shows the results of controlled modification of geometrical configuration and the physical and chemical properties of carbon based nanostructures, by laser direct writing.