AbstractThe realization of ferromagnetism in semiconductors is an attractive avenue for the development of spintronic applications. Here, we report a semiconducting layered metal-organic framework (MOF), namely K₃Fe₂[(2,3,9,10,16,17,23,24-octahydroxy phthalocyaninato)Fe] (K₃Fe₂[PcFe-O₈]) with spontaneous magnetization. This layered MOF features in-plane full π-d conjugation and exhibits semiconducting behavior with a room temperature carrier mobility of 15 ± 2 cm² V⁻¹ s⁻¹ as determined by time-resolved Terahertz spectroscopy. Magnetization experiments and ⁵⁷Fe Mössbauer spectroscopy demonstrate the presence of long-range magnetic correlations in K₃Fe₂[PcFe-O₈] arising from the magnetic coupling between iron centers via delocalized π electrons. The sample exhibits superparamagnetic features due to a distribution of crystal size and possesses magnetic hysteresis up to 350 K. Our work sets the stage for the development of spintronic materials exploiting magnetic MOF semiconductors.