Recording high quality biosignals by dry textile electrodes is a common challenge in medical health monitoring garments. The aim of this study was to improve skin–electrode interface and enhance the quality of recorded electrocardiography (ECG) signals by modification of textile electrodes embedded in WearItMed smart garment. The garment has been developed for long-term health monitoring in patients suffering from epilepsy and Parkinson’s disease. A skin-friendly electro-conductive elastic paste was formulated to coat and modify the surface of the knitted textile electrodes. The modifications improved the surface characteristics of the electrodes by promoting a more effective contact area between skin and electrode owing to a more even surface, fewer pores, greater surface stability against touch, and introduction of humidity barrier properties. The modifications decreased the skin–electrode contact impedance, and consequently improved the recorded ECG signals obviously when low pressure was applied to the electrodes, therefore contributed to greater patient comfort. The created contact surface allowed the natural humidity of the skin/sweat to ease the signal transfer between the electrode and the body, while introducing a shorter settling time and retaining moisture over a longer time. Microscopic images, ECG signal measurements, electrode–skin contact impedance at different pressures and times, and water absorbency were measured and reported.