The crystallization behavior of long-chain branched (LCB) poly(L-lactide) (PLLA), which were successfully prepared by successive functional group reactions, was studied by nonisothermal and isothermal methods in a wide temperature range. The density of the nuclei for LCB samples during crystallization was much higher than that for linear PLLA. According to qualitative information about the chain topologies of the branched PLLAs, obtained by a combination of linear viscoelasticity and branch-on-branch (BOB) dynamic modeling, it should be the backbones of LCB that are able to act as nuclei and thus markedly enhance the crystallization rate of PLLA. Moreover, a kinetic analysis of crystallization was performed using secondary nucleation theory.