Chrysanthemum ( Ramat.) is a seasonal plant with high medicinal and aesthetic value, and drying is an effective practice to enhance its storability after harvesting. The effects of hot air drying (HAD), combined infrared and hot air drying (IR-HAD), and sequential IR-HAD and HAD (IR-HAD + HAD) on the drying behavior, color, shrinkage, aroma profiles, phenolic compounds, and microstructure of chrysanthemum cakes were studied. Results showed that the increasing temperature resulted in a decrease in drying time and an increase in drying rate and moisture diffusivity. The Logarithmic and Page models exhibited superior fit in describing the dehydration process. Among the three drying strategies, IR-HAD was more effective in reducing energy consumption, improving shrinkage, water holding capacity, water binding capacity and cellular microstructure, while IR-HAD + HAD showed better inhibitory effect on color deterioration. Furthermore, gas chromatography-mass spectrometry (GC-MS) analysis revealed that different drying strategies dramatically influenced the aroma profiles in samples, and IR-HAD obtained the highest concentration of volatiles. The results of ultra-performance liquid chromatography (UPLC) indicated that the introduction of infrared radiation contributed to increasing the contents of chlorogenic acid, luteolin, total phenolic and flavonoid. These suggested that IR-HAD was a promising technique for drying medicinal chrysanthemum.