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It is an effective method to explore the full spectrum responsive photocatalysts for enhancing their photocatalytic activity. Herein, we have combined the upconversion phosphor with semiconductor to design the full‐spectrum light responsive photocatalyst. A facile approach has been developed for synthesis of NaYF4:Yb,Tm@TiO2 core‐shell structured composite. The morphologies, crystal phases, chemical compositions, optical performance, and photoelectric properties were characterized. Based on SEM and TEM observation, the formation mechanism of NaYF4:Yb,Tm@TiO2 composite was discussed in detail. The results of photodegradation experiment showed that 22% of Rhodamine B dye in the solution was photodegradated by NaYF4:Yb,Tm@TiO2 composite under NIR light irradiation within 150 min, suggesting that the NaYF4:Yb,Tm@TiO2 core‐shell structured composite displayed photocatalytic activity under NIR light irradiation. Furthermore, the photocatalytic ability of NaYF4:Yb,Tm@TiO2 is obvious superior to that of TiO2 under the full‐spectrum light irradiation. [ABSTRACT FROM AUTHOR]