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However, the clinical translation of conventional PDT remains limited by nonspecific activation, poor selectivity, and off-target phototoxicity. The dynamic and heterogeneous tumour microenvironment (TME)- defined by anomalous pH, elevated Glutathione (GSH) levels, malfunctioned redox homeostasis, enzyme overexpression, and irregular vascularization, which thus offers an opportunity to engineer next-generation photosensitizers that respond selectively to these cancer-specific stimuli. This review aims to explore recent advances in stimuli-responsive and theranostic cyclometalated iridium(III) systems designed to achieve anticancer activity in a spatiotemporal manner. We discuss the molecular design principles and mechanistic bases of TME-, redox-, enzyme-, and light-triggered activation, along with emerging multi-stimuli architectures that enhance the robustness in complexes. The review further focuses on the way Ir(III) Complexes unite therapy and diagnostics. Due to their inherent luminescence, redox characteristics, and excited-state behaviour, these complexes enable simultaneous imaging, ROS production, microenvironment sensing, and real-time monitoring of treatment responses. By correlating structural features with activation pathways and biological outcomes, the review seeks to provide a mechanistic framework for designing smart Ir(III)-based PDT agents with improved selectivity, reduced systemic toxicity, and enhanced therapeutic precision.<\/jats:p>","DOI":"10.1093\/mtomcs\/mfag021","type":"journal-article","created":{"date-parts":[[2026,6,15]],"date-time":"2026-06-15T22:55:37Z","timestamp":1781564137000},"source":"Crossref","is-referenced-by-count":0,"title":["Smart cyclometalated iridium photosensitizers: stimuli-responsive and theranostic systems for precision phototherapy"],"prefix":"10.1093","volume":"18","author":[{"given":"Sreejani","family":"Ghosh","sequence":"first","affiliation":[{"name":"Department of Chemistry, School of Advanced Sciences, Vellore Institute of Technology , Vellore 632014 Tamil Nadu 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