Metal-organic　frameworks　(MOFs)　have　recently　gained　extensive　attention　as　potential　materials　for　direct　radiation　detection　due　to　their　strong　radiation　absorption,　long-range　order,　and　chemical　tunability.　However,　it　remains　challenging　to　develop　a　practical　MOF-based　X-ray　direct　detector　that　possesses　high　X-ray　detection　efficiency,　radiation　stability,　and　environmental　friendliness.　The　integration　of　donor-acceptor　(D-A)　pairs　into　crystalline　MOFs　is　a　powerful　strategy　for　the　precise　fabrication　of　multifunctional　materials　with　unique　optoelectronic　properties.　Herein,　a　new　lead-free　MOF,　Cu2I2(TPPA)　(CuI-TPPA,　TPPA　=　tris[4-(pyridine-4-yl)phenyl]amine),　with　a　6-fold　interpenetrated　structure　is　designed　and　synthesized　based　on　the　electron　donor-acceptor　strategy.　CuI-TPPA　has　a　large　mobility-lifetime　(μτ)　product　of　5.8　×　10-4　cm2　V-1　and　a　high　detection　sensitivity　of　73.1　μC　Gyair-1　cm-2,　surpassing　that　of　commercial　α-Se　detectors.　Moreover,　the　detector　remains　fairly　stable　with　only　a　2%　reduction　in　photocurrent　under　continuous　bias　irradiation　conditions　with　a　total　dose　of　over　42.83　Gyair.　The　CuI-TPPA/poly(vinylidene　fluoride)　flexible　composite　X-ray　detector　films　are　successfully　manufactured　with　different　thicknesses.　Through　multifaceted　assessments,　the　optimal　thickness　is　found　with　a　high　detection　sensitivity　of　up　to　143.6　μC　Gyair-1　cm-2.　As　proof-of-concept,　11　×　9　pixelated　X-ray　detectors　are　fabricated　on　the　same　composite　film　to　realize　X-ray　direct　imaging.　This　work　opens　up　potential　applications　of　MOFs　in　environmentally　friendly　and　wearable　devices　for　direct　X-ray　detection　and　imaging.　©　2024　American　Chemical　Society.