The effectiveness of the optical rotation prediction (ORP) basis set for computing specific rotations at the coupled cluster (CC) level has been evaluated for a test set of 14 chiral compounds. For this purpose, the ORP basis set has been developed for the second-row atoms present in the investigated systems (that is, for sulfur, phosphorus, and chlorine). The quality of the resulting set was preliminarily evaluated for seven molecules using time-dependent density-functional theory (TD-DFT). Rotations were calculated with the coupled cluster singles and doubles method (CCSD) as well as the second-order approximate coupled cluster singles and doubles method (CC2) with the correlation-consistent aug-cc-pVDZ and aug-cc-pVTZ basis sets and extrapolated to estimate the complete basis-set (CBS) limit for comparison with the ORP basis set. In the compounds examined here, the ORP calculations on molecules containing only first-row atoms compare favorably with results from the larger aug-cc-pVTZ basis set, in some cases lying closer to the estimated CBS limit, while results for molecules containing correlation-consistent basis sets are necessary to obtain reliable estimates of the CBS limit.