The crystallization behavior of intercalated Poly(L-lactide) (PLLA)/organo-modified montmorillonite hybrids has been investigated in term of growth of spherulites and bulk crystallization. The PLLA hybrids were prepared via melt-compounding between PLLA and montmorillonite organo-modified (organoclay) with two different types of ammonium salts: trimethyl octadecyl- or bis(4-hydroxy butyl) methyl octadecyl ammonium salts. The nucleation rate of PLLA crystallites is slightly enhanced by natural clay, while reduced by organoclay due to the shielding effect and/or miscibility between surfactants of clays and PLLA chains. The incorporation of small amount of organoclay in PLLA matrix shows a tendency to reduce slightly the growth rate and the overall crystallization rate of PLLA crystallites. The secondary nucleation theory was utilized to discuss the crystallization behavior of these hybrids.