The recent discovery of hydrovoltaic devices for power generation has led to a rapid growth into new materials for harvesting energy specifically for this research field. Of the materials investigated, carbon materials have dominated, and graphene oxide (GO) has emerged as the leader. While graphite is conductive, it does not have functional groups to strongly interact with water, and highly functionalized GO forms strong interaction with water to generate necessary surface charges but does not typically have high conductivity. Herein, we report the fabrication and functionalization of a graphite-based structure, controlling the extent of oxidation to balance the effects of conductivity and functionalization to achieve high power outputs in hydrovoltaics. Devices prepared using the functionalized graphite achieve a power output of 53.3 μW/g. High power output and good film stability are key advances toward the practical application of hydrovoltaic devices for renewable energy.