Phototheranostic agents have thrived as prominent tools for tumor luminescence imaging and therapies. Herein, a series of organic photosensitizers (PSs) with donor‐acceptors (D‐A) are elaborately designed and synthesized. In particular, PPR‐2CN exhibits stable near infrared‐I (NIR‐I) emission, excellent free radicals generation and phototoxicity. Experimental analysis and calculations imply that a small singlet‐triplet energy gap (ΔES1−T1) and large spin‐orbit coupling (SOC) constant boost the intersystem crossing (ISC), leading to type‐I photodynamic therapy (PDT). Additionally, the specific glutamate (Glu) and glutathione (GSH) consumption abilities of PPR‐2CN inhibit the intracellular biosynthesis of GSH, resulting in redox dyshomeostasis and GSH‐depletion causing ferroptosis. This work first realizes that single component organic PS could be simultaneously used as a type‐I photodynamic agent and metal‐free ferroptosis inducer for NIR‐I imaging‐guided multimodal synergistic therapy.