To implement 2D molybdenum disulfide (MoS₂) in the flexible electronic industry, large, uniform, and crystalline films on flexible substrates are needed. Thermal atomic layer deposition (ALD) generates large-area uniform MoS₂ films at low temperatures directly on temperature-sensitive substrates. But if the grown films are amorphous, a high-temperature posttreatment of the whole sample, which may cause thermal degradation of the substrate or other layers, needs to be avoided. In this article, the crystallization of amorphous MoS₂ layers deposited by thermal ALD processed with picosecond laser pulses (λ = 532 nm), in a “cold” annealing process, is reported. The laser fluence range varies from (Formula presented.) = 8.73 mJ cm⁻² to (Formula presented.) = 18.25 mJ cm⁻² with scanning speeds from (Formula presented.) = 240 mm s⁻¹ to (Formula presented.) = 2640 mm s⁻¹. The crystallization and the influence of the processing parameters on the film morphology are analyzed in detail by Raman spectroscopy and scanning electron microscopy. Furthermore, a transition of amorphous MoS₂ by laser annealing to self-organized patterns is demonstrated and a possible process mechanism for the ultrashort-pulsed (usp)-laser annealing is discussed. Finally, the usp laser annealed films are compared to thermally and continuous-wave-laser-annealed samples.