Flexible, dry skin electrodes represent a potentially superior alternative to standard Ag/AgCl metal electrodes for wearable devices used in long-term monitoring. Herein, such electrodes were formed using a facile method for dispersing carbon nanotubes (CNTs) in a silicone matrix using custom amphiphilic dispersive additives (DSPAs). Using only brief mixing and without the use of solvents or surface modification of CNTs, 12 poly(ethylene oxide)-silanes (PEO-SAs) of varying cross-linkability, architecture, siloxane tether length, and molar ratio of siloxane:PEO were combined with an addition cure silicone and CNTs. Nearly all PEO-SA-modified silicone−CNT composites demonstrated improved conductivity compared to the unmodified composite. The best conductivities correlated to composites prepared with PEO-SAs that formed micelles of particular sizes (d of ∼ 200−300 nm) and coincided to PEO-SAs with a siloxane:PEO molar ratio of ∼0.75−3.00. Superior dispersion of CNTs by such PEO-SAs was exemplified by scanning electron microscopy. Advantageously, modified composites retained their moduli, rather than becoming more rigid. Resultant electrodes fabricated with modified composites showed skin-electrode impedance comparable to that of Ag/AgCl electrodes. Combined, these results demonstrate the potential of silicone−CNT composites prepared with PEO-SA DSPAs as flexible, dry electrodes as a superior alternative to traditional electrodes.