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Pound cake is one of the most consumed fine pastries all over the world. Especially for cake manufacturing, the rate of cake firming is a key factor which, along with microbiological considerations, dictates shelf life. Next to the ingredients, it is assumed that the rate of cake firming is mainly determined by the storage conditions, as well as the resultant effect on the microstructural orientation of the ingredients. However, detailed knowledge is still missing concerning changes in the major structural components of cakes (proteins, starch and lipids) during storage (e.g., molecular mobility, recrystallization) and their relation to cake firming rate. To characterize the influence of storage conditions on the structural components of cake, rheological and microstructural investigations at different storage temperatures (7; 14; 21; 28; 35 °C) were performed over 21 days. Lipid drop size distribution was visualized by confocal laser scanning microscope and analyzed with image processing software ImageJ. Crumb hardness measurements during storage were performed by TPA. In contrast to bread crumb, an increase in temperature leads to an increase in crumb hardness by more than 65% after 21 days. Inter alia, this effect accounts to starch recrystallization. Furthermore, area fraction analysis of lipids shows differences between the top (28%) and bottom (32%) of a cake cross section stored at 37 °C of about 4%, whereas no significant differences are observed at a storage temperature of 5 °C. The results reveal structural differences on cake firming and prove the influence of temperature and time on the major structural components. This study examined structural and textural changes in pound cakes stored at different temperatures, paying particular attention to the role of especially starch and lipids in cake firming.