Due to the copious development of industries and depletion of fossil fuels generate deteriorating environmental pollution and appalling economic crisis. Thus, there are increasing unmet for developing well-defined nanostructures to mitigate energy and environmental issues. Herein, we firstly report a unique concerted method to convert agro bio-waste into an economical wealth material. By the inspiration of nature, we selected a waste 2D garlic husk (Allium sativum) as a torchbearer to make a unique material. The garlic extract was applied for the synthesis of Fe₃O₄ NAs@2D-CCS composite nano-assemblies (NAs). Interestingly, the small-sized Fe₃O₄ nanocrystals (<20 nm) underwent nucleation in the presence of biogenic 2D-CCS and formed a pomegranate like a cluster (200 nm) forming a conglomerate on porous carbon layers. Most importantly, no secondary waste was generated in this work. This Fe₃O₄ NAs@2D-CCS composite affords high specific capacitance of 820F g⁻¹ at a current density of 0.5 A g⁻¹, which is nearly 5 to 3 times higher than pristine Fe₃O₄ NPs (<20 nm) electrode with an outstanding power density (3500–8000 W kg⁻¹) and specific energy density (115.5 to 65.9 Wh Kg⁻¹), which is superior among most of all reported iron oxide and graphitic carbon composites. This simple work stimulates a new door for the generation of waste to well-defined nanostructure materials for energy, catalysis, and environmental applications.