Graphene nanoscrolls (GNS) are 1D carbon-based nanoparticles. In this study, they were investigated as a heterogeneous nucleating agent in the poly(lactic acid) (PLA) matrix. The isothermal and non-isothermal melting behavior and crystallization kinetics of PLA-GNS nanocomposites were investigated using a differential scanning calorimeter (DSC). Low GNS content not only accelerated the crystallization rate, but also the degree of crystallinity of PLA. The Avrami model was used to fit raw experimental data, and to evaluate the crystallization kinetics for both isothermal and non-isothermal runs through the nucleation and growth rate. Additionally, the effect of the dimensionality and structure of the nanoparticle on the crystallization behavior and kinetics of PLA is discussed. GNS, having a similar fundamental unit as CNT and GNP, were observed to possess superior mechanical properties when analyzed by the nanoindentation technique. The scrolled architecture of GNS facilitated a better interface and increased energy absorption with PLA compared to CNTs and GNPs, resulting in superior mechanical properties.