This Perspective provides a current survey on the synthesis, self-assembly, and vast variety of applications possible from block copolymer (BCP) systems containing at least one segment of either poly(2-vinylpyridine), P2VP, or poly(4-vinylpyridine), P4VP. Strategies and insight toward P2VP or P4VP as the segment of choice and their influence on material properties, effective interaction parameters, and hosting a variety chemistries from small molecules to nanoparticles are provided. It is with hope that this work serves as a modern field guide to the versatility and utility of these chemistries for those new to or continuing research with these BCP systems.