The phenomenon of droplet coalescence and jumping has received increasing attention due to its potential applications in the fields of condensation heat transfer and surface self-cleaning. Basic research on the process and mechanism of coalescence-induced droplet jumping has been carried out, and some universal laws have been established. However, it is found that the focus of these studies is based on two identical droplets, and the coalescence-induced jumping with different radii is rarely investigated, which is commonly encountered in nature. Therefore, it is essential to proceed with the research of coalescence and jumping of droplets with unequal radii. In this paper, molecular dynamics (MD) simulations are performed to reveal the effects of radius ratio and radius of small droplets on jumping velocity. The results show that as the increasing of radius ratio with an unchanged small droplet radius of 8.1 nm, the jumping velocity increases then decreases, which indicates there is an optimal radius ratio to maximize the jumping velocity. Additionally, it is found that if the small droplet radius is changed, the critical radius ratio for characterizing whether the coalesced droplet jumping increases with increasing the small droplet radius. Furthermore, according to energy conservation, the conversion efficiency of energy is discussed. The results show that when the radius ratio is greater than 1.3 with three different small droplet radii, the energy conversion efficiency rapidly decreases to below 1.0%; and the critical radius ratios are consistent with the result obtained from the velocity analysis. This work broadens the understanding of the more general phenomenon of coalescence-induced droplet jumping and can better guide industrial applications.