Recently, there has been substantial interest in the large-scale synthesis of hierarchically architectured transition metal dichalcogenides and designing electrodes for energy conversion and storage applications such as electrocatalysis, rechargeable batteries, and supercapacitors. Here we report a novel hybrid laser-assisted micro/nanopatterning and sulfurization method for rapid manufacturing of hierarchically architectured molybdenum disulfide (MoS2) layers directly on molybdenum sheets. This laser surface structuring not only provides the ability to design specific micro/nanostructured patterns but also significantly enhances the crystal growth kinetics. Micro and nanoscale characterization methods are employed to study the morphological, structural, and atomistic characteristics of the formed crystals at various laser processing and crystal growth conditions. To compare the performance characteristics of the laser-structured and unstructured samples, Li-ion battery cells are fabricated and their energy storage capacity is measured. The hierarchically architectured MoS2 crystals show higher performance with specific capacities of about 10 mAh cm-2, at a current rate of 0.1 mA cm-2. This rapid laser patterning and growth of 2D materials directly on conductive sheets may enable the future large-scale and roll-to-roll manufacturing of energy and sensing devices.