In the current work, nanostructured pearlitic steels in bulk with interlamellar spacing of 86 and 168 nm, respectively, are developed through suitable alloying combined with appropriate heat treatment. The specimens extracted from the steels are tested separately in tension and torsion. Under tensile extension, finer pearlite shows a higher yield strength and ultimate tensile strength but fractures at a lower value of strain. However, under torsion testing, finer pearlite deforms to higher shear stress while fracturing at marginally larger shear strain than the coarser pearlite. Under torsion loading, the fractured surface of the finer pearlite presents a larger length of ductile crack propagation (DCP) extending from the circumference toward the center before initiation of cleavage fracture. Scanning electron microscopy (SEM) images of the DCP region are used to characterize the deformation of cementite lamellae, whereas electron backscattered diffraction (EBSD) maps reveal the misorientation changes in ferrite due to torsion. A more frequent and irregular change in ferrite misorientation for coarser pearlite in the DCP region is observed compared with finer pearlite. Bending and fragmentation of cementite lamellae are observed to be higher for fine pearlite, suggesting better strain accommodation. Thus, decreasing the lamellar spacing in nanostructured pearlite improves the torsional response.