Powdering whole lychee fruit is one of the most effective methods for improving the comprehensive utilization rate of lychees. In this study, lychee whole fruit powder (LWFP) was prepared and treated with low-temperature plasma, microwave, and 60Co γ-irradiation treatments to enhance its quality. Volatile organic compounds (VOCs) were analyzed using Headspace Solid Phase Micro-extraction Gas Chromatography-mass Spectrometry (HS-SPME-GC-MS), Headspace Gas Chromatography Ion Mobility Spectrometry (HS-GC-IMS), and electronic nose (E-nose) techniques. Electronic tongue (E-tongue) analysis revealed that both sweetness and bitterness were significant taste indicators of LWFP. GC-MS analysis revealed that the predominant volatile compounds in LWFP were terpenoids and alcohols, specifically nerol, geraniol, ɑ-pinene, hexylbenzene, ɑ-caryophyllene, caryophyllene oxide, and isoamylenol. GC-IMS identified small-molecule aldehydes such as 2-methyl propanal, hexanal, propanal, and 2-methylbutanal as significant contributors to the aroma profile. Moreover, key aromatic contributors include dimethyl sulfide, 1-penten-3-one, and acetic acid. Notably, microwave treatment exerted the most significant effect on the aroma profile of lychee. In contrast, low-temperature plasma and irradiation treatments exhibited similar and consistent changes. Specifically, microwave treatment primarily increased the concentration of larger terpenoid molecules such as nerol, 1-phenylhexane, and caryophyllene oxide, whereas low-temperature plasma and irradiation had a greater impact on smaller aldehyde molecules such as hexanal and 2-methylbutanal. All treatments enriched the sweet fruity, brilliant woody, and cabbage scents of LWFP.