Metal-organic framework (MOF) derivatives have drawn considerable attention for applications in various fields. In this work, spindle-shaped Ce-TCPPs were assembled by a rapid microwave-assisted hydrothermal method. After thermal treatment at low temperature under a N atmosphere, the Ce-TCPPs were partially pyrolyzed and converted to a novel CeO/N-doped carbon/Ce-TCPP nanocomposite. Compared to completely decomposed materials, these partially decomposed heterogeneous catalysts exhibited significantly higher photocatalytic activation ability toward PMS for the removal of organic pollutants (e.g., rhodamine B, methylene blue, methyl orange, tetracycline and oxytetracycline). For the optimized sample thermal treated at 450 °C, a 100 mL RhB solution (10 mg/L) can be removed within 20 min with the assistance of PMS under visible light. The significantly enhanced activity can be attributed to the effective spatial separation of photogenerated electrons and holes in the formed Z-scheme CeO/N-doped carbon/Ce-TCPP system. This work may provide useful guidance for the design and fabrication of MOF-derived photocatalytic systems for environmental remediation.