Here, a well crystalline 3D flower-like structured MoS2 (~420 nm) has been successfully synthesized on a large scale by a simple hydrothermal technique. The evolution of morphology in the formation process has also been investigated. The crystallinity, purity, and morphology of the sample are characterized by powder X-ray diffraction, Fourier-transform infrared spectroscopy, fieldemission scanning electron microscopy (FESEM), and transmission electron microscopy (TEM) techniques. The FESEM and TEM images reveal that the sample exhibits a uniform 3D flower-like microsphere shape with folded nanosheets, which are stretched out along the edge of the microsphere. The electrochemical performance of the sample has been investigated by cyclic voltammogram, galvanostatic charge–discharge, and electrochemical impedance spectroscopy studies. The results of the electrochemical analysis suggest that the material delivers a maximum specific capacitance (Csp) of 350 F/g at a discharge current density of 0.25 A/g with energy density 17.5 Wh/kg. It also exhibits good capability and excellent cyclic stability (94% capacity retention after 1,000 cycles in 1 A/g) owing to the coupling effect of electrical conductivity with the interesting morphology and larger active surface area. Hence, the sample may be used as a promising electrode material for high-performance energy storage devices.