In this paper, the effects of different proteins (soybean protein isolate, wheat protein hydrolysate, tremella protein) on the activity of tremella polysaccharide under different conditions were studied. The optimal protein-polysaccharide complex was determined by grafting degree and activity screening, and the microstructure and rheological properties were studied. The results showed that when the ratio of soybean protein isolate to tremella polysaccharide was 2:1 and the solution pH was 7, the optimal complex was obtained by heating at 90 °C for 4 h, and its grafting degree and antioxidant activity were the best. Studies have shown that tremella polysaccharide and soybean protein isolate complex (TFP-SPI) solution is pseudoplastic fluids. At the same time, tremella polysaccharide (TFP) and TFP-SPI were used for electrospinning to observe its spinnability. When the ratio of PVA/TFP-SPI/PL was 8:1:1, nanofibers with uniform diameter and good morphology were obtained. This paper provides a theoretical basis for the comprehensive utilization of tremella polysaccharide and its electrospun fiber can be used as active film for food packaging.