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We report on the rational synthesis of coiled carbon nanotube (CNT) and nanowires morphologies, through chemical vapor deposition, made feasible through extensive thermodynamic analysis and modeling. Coil formation is scientifically interesting in that helices abound in nature, e.g., DNA, proteins, etc., and a connection is being made at the nanoscale between carbon based inorganic and organic forms. Such morphologies can be used in a wide variety of applications, e.g., nanoscale electrical inductors and mechanical springs. We have also shown that polymer composites constituted of such helical forms exhibit a greater electromagnetic interference (EMI) shielding efficiency compared to composites constituted from the linear CNTs.