Considering the increasing demand for advanced energy materials for future energy-related applications, designing promising materials at a low cost is critical. Given the importance of structural design and morphological features of the designed material in energy applications, fabricating materials at the nanoscale with controlled morphology and orientation is important. Recently 2-dimensional graphene-based materials have emerged as a potential candidate for next-generation energy applications. However, conventional chemical and physical routes for producing high-quality graphene have certain limitations either due to the cost or the processing time. Therefore, an advanced technique for designing and processing graphene structures at the atomic scale is needed to produce high-quality materials. In this regard, safe and clean environmentally-friendly plasma-enabled techniques have been explored as a potential method to tailor different structures at the nanoscale. As a synthesis approach, plasma assembles the nanostructures from gaseous into a solid form. Therefore, this paper suggests the advantages of atmospheric pressure plasma-enabled approaches to design and engineer graphene-based materials at the nanoscale with high structural quality and controllability with hybrid morphologies. Here, a novel, single-step microwave plasma-enabled approach at atmospheric conditions used to design hybrid high-quality graphene-based nanostructures is presented. The plasma techniques allow the synthesis of high-quality N-graphene (nitrogen-doped graphene) metal-based nanostructures at one of the fastest production rates of ∼ 19 mg/min. The graphene production is carried out in the high energy density zone of microwave plasma, and the growth of N-graphene sheets occurred in the afterglow region. Spraying metal particle-containing gases into this zone allows the formation of hybrid N-graphene structures anchored with metal oxide/sulphide nanoparticles. Structural and morphological analysis of these hybrids using different microscopic and spectroscopic techniques confirmed the high structural quality and distribution of metal-based nanostructures on N-graphene sheets. This fast and facile approach is expected to provide a significant impact on designing high-quality graphene hybrids, which can be used for sustainable energy storage applications.