Organic photodiodes (OPDs) are a significant focus for the next-generation of light-detection technologies. However, organic semiconductors in OPDs still face key challenges, such as low carrier mobilities and limited efficiency in generating photon-induced signals, which affect the detectable resolution and dynamic range. In this study, the characterization of the interaction between organic polymeric bulk heterojunctions and two-dimensional (2D) transition metal dichalcogenides (MoS2) reveals an enhancement in photocurrent due to improved photogeneration dynamics (e.g., reduction of bimolecular recombination and enhancing charge carrier transfer). Consequently, the optimized 2D MoS2-additive OPD achieved an exceptionally high linear dynamic range (LDR) exceeding 174 dB and an outstanding specific detectivity (D*) of 3.21 × 1012 Jones, while reaching femto-scale noise levels. This presents the potential of state-of-the-art OPDs for various light signal applications.