This review explores the diverse applications of polyvinylidene fluoride (PVDF) and carbon nanomaterials (CNMs) systems, highlighting their use in electromagnetic interference (EMI) shielding, piezoelectrics, and various sensing modalities. The materials are also effective in biomaterials, such as tactile skin and COVID-preventing facemasks through sunlight sterilization. Additionally, PVDF-CNMs excel in radar absorption, solar-assisted electricity generation, triboelectric energy harvesting, 3D-4D printing materials, anti-icing covers, anti-stealth materials, and heat-dissipating solids in electronics. The research integrates materials chemistry and engineering, aiming to synthesize insights from fundamental sciences and technologies. The review focuses on the structural attributes and physicochemical properties of PVDF and CNMs, particularly the conversion from PVDF α- to β-phase, which enhances its applicability in EMI shielding, piezoelectrics, sensors, and energy harvesters. The simplicity of generating PVDF-CNMs and their potential for tuning material features like hydrophilicity, mechanical properties, piezoelectric characteristics, catalytic activity, and bioactivity is also discussed. The pursuit of scientific excellence in this field indicates new avenues for discovery and innovation.This review explores the diverse applications of polyvinylidene fluoride (PVDF) and carbon nanomaterials (CNMs) systems, highlighting their use in electromagnetic interference (EMI) shielding, piezoelectrics, and various sensing modalities. The materials are also effective in biomaterials, such as tactile skin and COVID-preventing facemasks through sunlight sterilization. Additionally, PVDF-CNMs excel in radar absorption, solar-assisted electricity generation, triboelectric energy harvesting, 3D-4D printing materials, anti-icing covers, anti-stealth materials, and heat-dissipating solids in electronics. The research integrates materials chemistry and engineering, aiming to synthesize insights from fundamental sciences and technologies. The review focuses on the structural attributes and physicochemical properties of PVDF and CNMs, particularly the conversion from PVDF α- to β-phase, which enhances its applicability in EMI shielding, piezoelectrics, sensors, and energy harvesters. The simplicity of generating PVDF-CNMs and their potential for tuning material features like hydrophilicity, mechanical properties, piezoelectric characteristics, catalytic activity, and bioactivity is also discussed. The pursuit of scientific excellence in this field indicates new avenues for discovery and innovation.