The mulberry fruit is edible and medicinal, and it is commonly referred to as the “best health product of the 21st century”. The purpose of this study was to find out whether different drying methods affect the quality of mulberry fruits and the main nature of the volatile organic compounds (VOCs) they contain. This study used vacuum freeze-drying (VFD), vacuum drying (VD), sun drying (SD), hot-air drying (HAD), and microwave drying (MD) to treat fresh mulberry fruits. Gas-phase ion mobility spectrometry (GC-IMS) was used to detect and analyze the VOCs in mulberry fruit samples treated with the different drying methods. There were 47 VOCs detected, with aldehydes and alcohols dominating. The obtained data were subjected to principal component analysis (PCA), cluster analysis (CA), nearest neighbor fingerprint analysis, and partial least-squares regression analysis (PLS-DA). The conclusion was drawn that fresh mulberry fruits contain abundant VOCs, and mulberry fruits after VD contain many aldehydes; thus, VD promoted the synthesis of phellandrene and other compounds widely used in the preparation of cosmetics such as perfume and soap. HAD promoted the synthesis of esters commonly used in the preparation of fruit flavor and wine essence. The higher (E)-2-heptenal content with SD was conducive to the Maillard reaction. MD promoted the synthesis of heptanal and valeraldehyde with aroma characteristics such as fatty, green, fruity, grassy, and floral. According to the VIP results, VOCs (E)-2-heptenal, pentanal D, cyclohexanone, and 2-hexanone D influenced the VOCs in most of the mulberry fruit samples. The findings of this study provide an important reference for drying mulberry fruits, which, in turn, will help to ensure the safety and effectiveness of processed mulberry fruit products.