The efficient removal of volatile organic compounds (VOCs) is still challenging, and suitable strategies and auxiliary materials are lacking. Herein, we propose a highly efficient and stable iron-based metal-organic framework (Fe-MOF) in which the adsorption removal and photodegradation regeneration step alternate to realize repeatable and efficient removal of VOCs. A group of morphology-controlled Fe-MOFs serves as both the adsorbent and photocatalyst under ambient conditions to remove typical VOCs, e.g., toluene by relying on their high porosity and catalytic activity. The optimized Fe-MOF exhibits 100% adsorption removal efficiency for a toluene concentration of 460 ppm, and the Fe-MOF could be regenerated by converting the adsorbed toluene into harmless CO₂ under 1 SUN (100 mW/cm²) solar irradiation. More importantly, the Fe-MOF showed excellent durability during repeated adsorption and degradation processes for 100 cycles.