Commercially available 4,4'-methylene bis(phenyl isocyanate), when copolymerized with the atropisomeric monomer S-(-)-1,1'-binaphthyl-2,2'-diamine, provides convenient access to urea-linked polymers that exhibit exceptional levels of solvent-dependent chiroptical behavior. The use of different solvent media affords a high degree of control over both the sign and magnitude of the optical rotations that are ultimately displayed by these conformationally dynamic systems. The polarity of the solvent environment appears to play a role in shaping polymer responses. A number of related poly(urea-amide) constructs fitted with azobenzene backbone segments are also sensitive to the application of light and heat, ultimately providing for highly adaptive material systems with chiroptical outputs that can be dynamically modulated in real-time by a combination of different input signals. (C) 2015 Elsevier Ltd. All rights reserved.