Research on the effect of ammonium chloride (NH₄Cl) electrolyte on graphene nanosheet (GNS) electrodes derived from candlenut shells (Aleurites moluccana (L.) Willd) as primary battery cathodes has been conducted. GNS was synthesized via pyrolysis and modified with NH₄Cl to produce G–N 0.5 M, G–N 1.0 M, G–N 2.0 M, and G–N 3.0 M samples. The materials were characterized using XRD, SEM-EDX, and electrical measurements at 0.5–1.5 V. XRD results show peaks at 2θ ≈ 25° and 44.27° corresponding to C(002) and C(100) planes, while G–N samples exhibit new diffraction peaks at (111), (200), (220), (311), (222), and (400), indicating NH₄Cl incorporation. SEM analysis reveals a transition from layered GNS morphology to more wrinkled and agglomerated structures with increasing NH₄Cl concentration, supported by EDX showing decreasing carbon content and the presence of chlorine (up to ~5.9%). Electrical conductivity increases significantly from commercial battery to GNS and further to G–N samples, reaching ~1.30 S·cm⁻¹ for G–N 2.0 M, along with energy density (~605 Wh·kg⁻¹) and power density (~605 W·kg⁻¹). These results indicate that NH₄Cl modification enhances electrochemical performance and highlights the importance of electrolyte variation in optimizing GNS-based electrodes for primary battery applications.