Activity-guided fractionation of seeds of Solanumindicumfor anti-HBV activity led to the isolation of two novel coumarinolignoid alkaloids (indicumines A–B, 1–2) and two newcoumarinolignoids (indicumines C–D, 3–4), together with four known coumarins (5–8). Their structures were established on the basis of spectroscopic data. The two novel coumarinolignoid alkaloids shows anti-HBV activities through specifically inhibiting the secretion of HBsAg in HepG2.2.15