This study investigates the integration of green- and red-emitting carbon dots into the MIL-53(Al) MOF, exploring the structural and optical properties and their impacts on photocatalytic capabilities regarding the photodegradation of the organic dye Rhodamine B. Both types of carbon dots significantly enhance the degradation efficiency, particularly the composites with neutral-red carbon dots at different pH levels. Furthermore, UV-vis absorption and time-resolved photoluminescence spectroscopies provide evidence of electronic structure modifications, such as the enhanced charge separation and the observation of new emission bands related to carbon dots. These findings agree with the structural and optical changes induced by carbon dots integration into the MIL-53(Al) MOF. In general, this research work elucidates the transformative potential of carbon dots and MOF-based composites for advanced material applications, including catalysis and environmental remediation.