Aloe vera‐derived graphene (ADG) coupled system photocatalyst, mimicking natural photosynthesis, is one of the most promising ways for converting solar energy into ammonia (NH3) and nicotinamide adenine dinucleotide (NADH) that have been widely used to make the numerous chemicals such as fertilizer and fuel. In this study, we report the synthesis of the aloe vera‐derived graphene‐coupled phenosafranin (ADGCP) acting as a highly efficient photocatalyst for the generation of NH3 and regeneration of NADH from nitrogen (N2) and oxidized form of nicotinamide adenine dinucleotide (NAD+). The results show a benchmark instance for mimicking natural photosynthesis activity as well as the practical applications for the solar‐driven selective formation of NH3 and the regeneration of NADH by using the newly designed photocatalyst. In this study, the utilization of solar light irradiation enables the generation and regeneration of ammonia and NADH using an aloe vera‐derived graphene‐coupled phenosafranin (ADGCP) photocatalyst. The results show the remarkable efficiency and environmental friendly nature of the ADGCP system, offering the promising way to solve worldwide issues related to sustainable chemical synthesis and energy production.