Water absorption is the dominant factor affecting the quality deterioration of dried Lentinus edodes. We therefore analyzed the effect of moisture content and dynamic water status on physical properties of the mushroom stored at water activity (aw), 0.33, 0.43, 0.67, 0.76, and 0.84 for 50 days. Moisture mobility and water status were analyzed using low‐field nuclear magnetic resonance, while hardness and microstructure were determined as texture characteristics. Meanwhile, an electronic nose and headspace solid‐phase micro‐extraction combined with gas chromatography–mass spectrometry (HS–SPME–GC–MS) were used to analyze the flavor properties of dried L. edodes. The results showed that bound water was the dominant water status in dried L. edodes. The content and molecular mobility of bound water increased at aw = 0.67, 0.76, and 0.84. This contributed to discoloration, hardness loss, and microstructure sparsity of dried L. edodes. The increasing content and molecular mobility of bound water aggravated the deterioration of characteristic flavor by reducing acid, aldehyde, and ketone content. Unlike immobilized or free water, bound water had a critical influence on the quality deterioration of dried L. edodes during storage.