Exploring novel versatile electrode materials with outstanding electrochemical performance is the key to the development of advanced energy conversion and storage devices. In this work, we aim to construct new-fangled one-dimensional(1D) quasi-layered patronite vanadium tetrasulfide(VS4) nanostructures by using different sulfur sources, namely thiourea, thioacetamide, and L-cysteine through an ethyleneaminetetraacetic-acid(EDTA)-mediated solvothermal process. The as-prepared VS4exhibits several unique morphologies such as urchin, fluffy nanoflower, and polyhedron with appropriate surface areas. Among the prepared nanostructures, the VS4-1@NF nanostructure exhibited excellent electrochemical properties in 6 M KOH solution, and we explored its redox electrochemistry in detail. The asprepared VS4-1@NF electrode exhibited battery-type redox characteristics with the highest capacity of280 C g-1in a three-electrode assembly. Moreover, it offered a capacity of 123 F g-1in a hybrid twoelectrode set-up at 1 A g-1with the highest specific energy and specific power of 38.5 W h kg-1and750 W kg-1, respectively. Furthermore, to ensure the practical applicability and real-world performance of the prepared hybrid AC@NF//VS4-1@NF cell, we performed a cycling stability test with more than 5,000galvanostatic charge–discharge cycles at 2 A g-1, and the cell retained around 84.7% of its capacitance even after 5,000 cycles with a CE of 96.1%.