<p>Wheat gluten is an insulator with plasticizer dependency, which limits its functional applications, such as its use in conductive devices. The current study addresses this issue by presenting a solvent-assisted, non-swelling, hydraulic compaction method that can promote the interfacial localization of carbon nanofillers, such as carbon black and carbon nanotubes, while preventing the main protein structure from being damaged. The prepared wheat gluten-based pellets were characterized thoroughly for their structural, morphological, and conductive parameters by four-point probe analysis, Fourier transform infrared spectroscopy, differential scanning calorimetry, scanning electron microscopy, energy-dispersive X-ray spectroscopy, zeta potential, and confocal laser scanning microscopy. The transition in electrical conductivity of prepared pellets appeared from an insulating (&lt; 10⁻⁹ S/cm) wheat gluten control to semiconducting (0.2283 ± 0.0013 to 0.6498 ± 0.0039 S/cm) hybrid systems and highly conductive (40.79 ± 2.3 S/cm) carbon nanotube-rich composite pellet. These findings demonstrate that microstructure-guided processing enables tunable charge transport in biodegradable protein matrices. This work will help future studies to explore long-term stability, mechanical performance, and device-level integration for sustainable bioelectronic applications.</p>