Biomolecules are exquisitely adept at molecular recognition and self-assembly, enabling them to direct all of the processes that make life possible. These capabilities have been fine-tuned by billions of years of evolution, and more recently, have been harnessed in the laboratory to enable the use of biomolecules for applications beyond their canonical biological roles. The common thread that is woven throughout our research program is the utilization of nucleic acid molecular recognition and self-assembly to generate functional architectures for biosensing and bioimaging. We have harnessed photoaffinity labeling to covalently tag specific RNA transcripts with small-molecule fluorophore, subsequently enabling visualization of RNA localization and dynamics in living cells. We have also demonstrated the modulation of EndoV activity to enable selective enrichment of inosine-containing RNAs, which has enabled the identification of new A-to-I editing sites.