Photocatalytic degrading pollutants driven by visible-light irradiation has attracted tremendous attention. One strategy of preparing carbonized cellulose nanofibrils/Ti3C2Tx MXene/g-C3N4 (CMCN) as a photocatalyst was developed. The as-prepared CMCN was comprehensively characterized in terms of the chemical composition, chemical and crystal structure, morphology, and photoelectrochemical properties. The CMCN was explored as a photocatalyst and exhibited good photocatalytic performance in degrading MB (96.5%), RhB (95.4%), and TC (86.5%) under visible-light conditions. In addition, the CMCN as a photocatalyst exhibited good reusability and stability. It is found that the incorporation of cellulose nanofibrils provided a high carbon content, a high porosity, and a large specific surface area, enhanced the electron transfer, improved the photocatalytic performance, and ensured a semiconductor with a high stability. It is believed that this study would provide an effective approach to preparing a photocatalyst and broaden the potential application of cellulose nanofibrils in photocatalysis.