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• Increased exploration of synthetic macrocycles for various advanced biomedical applications. • Polyazamacrocycles excel as ion sensors due to their interactions with cations and anions. • Macrocyclic complexes show potential in antimicrobial, antioxidant, and anti-cancer applications. • Detailed review of synthesis methods for macrocyclic Schiff base ligands with various metal ions. • Macrocyclic complexes offer significant potential as MRI contrast agents and DNA cleaving agents. In recent years, there has been a significant increase in the exploration of various features of new macrocyclic ligands and complexes. Synthetically developed macrocycles, such as gadodiamide and phthalocyanine complexes, mimic naturally occurring macrocycles and have numerous applications, including photochemical activity, dye-stuff production, and use as MRI contrasting agents and in other biomedical applications. Polyazamacrocycles have become particularly important due to their ability to interact with both cations and anions and their versatility as ion sensors. This current review describes the overview of non-template and template-mediated synthesis of macrocyclic Schiff base ligands and their complexes in the presence of transition and inner transition metal ions with their advanced range of biomedical applications. This detailed and contemporary review is specifically recapitulates the effectiveness of macrocyclic complexes as antimicrobial, antioxidant, and anti-cancerous as well as potential MRI contrast agents, DNA binders, and DNA cleaving agents. The diverse range of synthetic protocols is also delineated in this work. The practical and assuring potential in sensing area are comprehensively reviewed. This review will be supportive for researchers to establish new deliberations in the expedition for designing novel macrocyclic complexes for pharmaceutical and diagnostics purposes. [Display omitted] [ABSTRACT FROM AUTHOR]