Conductive hydrogels are promising for neuroregenerative therapy due to their flexibility and ability to support electrical signal transmission. This study develops a PPy/gelatine conductive hydrogel with optimized electrical properties. Gelatine, known for its biocompatibility, was combined with the conductive polymer PPy and crosslinked using glutaraldehyde. Hydrogels with varying PPy concentrations (0 wt%, 2 wt%, 4 wt%, and 6 wt%) were analyzed. FTIR confirmed chemical bonding between gelatine and PPy, while XRD showed an increased crystallinity index compared to the Gel/0PPy sample. Cyclic voltammetry revealed that a 6% PPy concentration markedly enhanced electrical reactivity compared to lower concentrations. Results indicate that the crosslinking network between PPy and gelatine enhances conductivity by facilitating π-electron mobilization in the PPy backbones through the increased order of crystallinity. Additionally, higher PPy concentrations better facilitate more efficient electron and ionic transport, significantly boosting the hydrogel’s electrical activity. Notably, our findings demonstrate that even with similar crystallinity percentages, a higher PPy concentration (6%) markedly enhances electrical activity compared to a lower concentration (4%). These results highlight the crucial importance of optimizing both the crosslinking network and PPy concentration to significantly improve the hydrogel’s electrical properties, which is essential for future use in electroactive materials.