One of the most significant current discussions on Pu-erh tea (ripe tea) is the unique aroma of aging, but the key aroma-presenting substance for aging is unclear. This paper explores the relationship between the aging aroma of Pu-erh tea (ripe tea) and the drying method after fermentation. Head space solid-phase microextraction and gas chromatography-mass spectrometry (HS-SPME-GC-MS) and odor activity value (OAV) analyzed the tea samples with different drying methods and temperatures. The results showed that 4-methoxystyrene, 1,2-dihydro-1,1,6-trimethyl-naphthalene, (-)-camphor, 6-vinyldihydro-2,2,6-trimethyl-2H-pyran-3(4H)-one and 1,2-dihydro-1,1,6-trimethyl-naphthalene were the key aroma components for aging and were influenced by the drying method and temperature. In the sensory evaluation, PEH (Dryer-dry) had a strong and persistent aging aroma, PES (Sun-dry) and PEY (Shade-dry) had strong aging with medicinal herb aroma, and PEY was better than PES and PEW (Microwave-dry) had a strong aroma. We can see that the different drying methods have a greater influence on the aroma of Pu-erh tea (ripe tea), with the best aging quality of Pu-erh tea (ripe tea) when dried at 60 °C degrees.