The design and synthesis of multifunctionalized, architecturally controlled polymers is a prerequisite for a variety of future applications of polymeric materials. On the basis of Nature's use of self-assembly in the creation of biomaterials, this Account describes concepts that were developed over the past 5 years that utilize noncovalent interactions such as hydrogen bonding, ionic interactions, electrostatic interactions, metal coordination, and pi-pi stacking in modification of copolymer side-chains to obtain multifunctional polymeric materials, induce polymer morphology changes, and influence bulk-polymer properties.