Conjugated microporous polymers (CMP) are advanced photocatalytic systems for degrading organic dyes. However, their potential and efficiency are often limited by rapid electron–hole pair (e−/h+) recombination. To overcome this limitation, this study proposes a strategy that involves designing a Mott–Schottky heterojunction and integrating graphene sheets with a near-zero bandgap into the CMP-1 framework, resulting in a non-covalent graphene/CMP (GCMP) heterojunction composite. GCMP serves two main functions: physical adsorption and photocatalytic absorption that uses visible light energy to trigger and degrade the organic dye. GCMP effectively degraded four dyes with both anionic and cationic properties (Rhodamine B; Nile Blue; Congo Red; and Orange II), demonstrating stable recyclability without losing its effectiveness. When exposed to visible light, GCMP generates reactive oxygen species (ROS), primarily singlet oxygen (1O