Camellia shells are the main by-product of camellia seed processing and are usually incinerated or disposed of as agricultural waste. In this study, camellia shells were employed in the Pleurotus pulmonarius cultivation process using five distinct formulae substituting for cottonseed shells. Our results show that as the substitution rate of camellia shells increased from 0% to 35%, the protein content in P. pulmonarius significantly increased from 34.05% to 53.35%. The polysaccharide content reached a peak value of 5.62% at 30% substitution of camellia shells. The DPPH free radical scavenging rate reached its maximum of 82.70% at 20% substitution of camellia shells. Furthermore, increases in the total amino acid contents in P. pulmonarius were positively correlated with the substitution rate of camellia shells. Considering the yield characteristics, the formula of 20% camellia shell substitution tested in this study appears to be optimal for P. pulmonarius cultivation. These findings not only provide a substrate to enhance the nutritional quality of P. pulmonarius but also demonstrate a novel approach for the ecological utilization of camellia shells.