The invention discloses a synergistically reinforced anti-tumor near-infrared photoresponsive NaYF4: Yb, Er-NH2/RBS/GO/BNN6 nanocomposites, NaYF4: Yb, Er-NH2 layer, NO donor RBS layer, GO layer, NO donor BNN6 layer. The NaYF4: Yb, Er-NH2/RBS/GO/BNN6 nanocomposites have good thermal stability and high near-infrared response. NO emission can be triggered and controlled effectively by the switching of near infrared laser, the adjustment of irradiation time and power density. NaYF4: Yb, Er and GO, NO donors RBS and BNN6 can play a synergistic role, greatly enhance the response to near-infrared light, can significantly improve the therapeutic effect of tumor, showing a synergistic enhancement of the anti-tumor effect.