Recent discoveries on the improved versatility of helical polycarbodiimides capable of undergoing low energy reversible conformational changes from realignment of their restricted polyarene pendant groups has led to seven new polycarbodiimides that each present unique information in regards to how the electronics and connectivity of the arene pi-system play a crucial role in the behavior of these polymers. In addition to their individual anomalous behavior, this series of functional polymers unlock new answers toward the global understanding of the governing forces behind this complex switching process. Through the incorporation of functional groups covalently attached to the naphthalene pendant, dramatic changes and new application of these systems are realized. Variable temperature polarimetry is used to observe the reversible conformational changes of these chiral polymers. (C) 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 49: 719-728, 2011