The large family of transition metal dichalcogenides (TMDCs) has recently emerged as an important class of materials for future flexible electronic, optoelectronic, and photonic applications due to their outstanding electrical, optical, and mechanical properties. The crystallization and patterning of 2D materials on flexible substrates such as Polydimethylsiloxane (PDMS) and polyimide are, therefore, important for fabricating the next-generation electronics and photonics devices. Flexible substrates such as PDMS are highly suitable for use in wearable and biomedical applications, which can comfortably wrap to the human body parts. Synthesis of 2D materials via conventional growth methods such as chemical vapor deposition (CVD) requires high processing temperatures (~800 °C) that are well beyond the tolerance of flexible substrates. Moreover, fabrication of electronic and phonics devices, such as field-effect transistors (FETs) and photonics waveguide, from these materials typically require multistep patterning steps, including lithography, etching, and transfer. The patterning steps can become economically expensive and time-consuming. Here we demonstrate a direct laser crystallization and pattering of large-area 2D quantum materials on flexible substrates to create complex electronic and photonic structures. Controlled crystallization and direct writing processes are achieved by a precise laser processing of the pulsed laser deposited stoichiometric amorphous 2D films on the flexible substrates. A tunable nanosecond fiber laser (1064nm) coupled to a galvo scanner system was used to create the desired crystalline pattern of 2D materials on the PDMS substrates. The influence of laser pulse duration, the number of pulses, and thickness of the deposited 2D amorphous layer on the crystallization of 2D materials are discussed. This laser crystallization method opens up new routes for the synthesis of 2D materials with complex shapes and patterns on flexible substrates.