Rainfall interception research in forest ecosystems usually focuses on interception by either tree crown or leaf litter, although the 2 components interact when rainfall occurs. A process‐based study was conducted to jointly measure rainfall interception by crown and litter and the interaction between the 2 interception processes for 4 tree species (Platycladus orientalis and Pinus tabulaeformis represented needle‐leaf species, and Quercus variabilis and Acer truncatum represented broadleaf species) at 3 simulated rainfall intensities (10, 50, and 100 mm hr−1). Results indicated that (a) crown and litter interception processes incorporated 3 phases: the dampening phase, the steady saturation phase, and the postrainfall drainage phase, but the dampening phase for litter interception usually lasted 30 min longer than for crown interception; (b) the maximum and minimum interception storage (Cmax and Cmin) for the crown were 0.63 and 0.36 mm on average, and litter Cmax and Cmin were 5.38 and 2.36 mm, respectively; (c) generally, crown and litter Cmax and Cmin increased when gross precipitation increased significantly (p < .05) from 10 to 100 mm; and (4) crown Cmax and Cmin for needle‐species were 1.8 and 1.2 times larger than broadleaf species, whereas broadleaf litter showed the opposite, its Cmax and Cmin were 2.0 and 1.6 times larger than needle‐leaf litter on average; however, no significant differences were observed in crown and litter Cmax and Cmin between species on per leaf area and litter thickness basis. Results were normalized by total leaf area and litter thickness to provide a way to scale up from young trees to mature forests. Overall, rainfall interception was affected by biotic and abiotic factors together and could be quantified via multiple linear regression functions.